Bioinspired supramolecular polymers with water-triggered dense domains: achieving mechanical robustness, programmability, and weather resistance

Bioinspired supramolecular polymers with water-triggered dense domains: achieving mechanical robustness, programmability, and weather resistance | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Article Bioinspired supramolecular polymers with water-triggered dense domains: achieving mechanical robustness, programmability, and weather resistance Dawei Zhao, Changhong Lin, Geyuan Jiang, Minxin Wang, Haipeng Yu This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-8305182/v1 This work is licensed under a CC BY 4.0 License Status: Under Review Version 1 posted You are reading this latest preprint version Abstract Human muscles enhance their mechanical strength through structural training for densification of cellular networks; however, challenges remain in incorporating this feature into synthetic materials. Here, we report a water-triggered supramolecular polymer composed of cellulose and polymethyl methacrylate that achieves over a 22-fold improvement in mechanical properties. During this bioinspired process, water molecules trigger the transition of a stretchable supramolecular network into a densified cross-linked domain. The resultant polymer exhibits a remarkable increase in tensile strength from 2.7 MPa to 61.7 MPa, and demonstrate a substantial flexural strength of 97 MPa, while maintaining impressive structural integrity across a temperature range of -196°C to 180°C. In addition, the polymers possess scalable water-shaping and reinforcement capability, even in seawater or textile wastewater, retaining 100% of their mechanical performance, which allows for customization into tailored geometric structures. Economic analysis and recycling assessment demonstrate that this polymer possesses successful scalability and considerable market. This study provides a biomimetic formulation for the fabrication of high-performance supramolecular polymers, broadening their applications across various fields. Physical sciences/Materials science/Soft materials/Polymers Physical sciences/Materials science/Nanoscale materials/Structural properties cellulose water-triggering supramolecular polymer shapeability weather resistance Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Figure 7 Introduction Muscle development directly influences an individual's strength and endurance 1 – 3 . Mechanical training can promote the thickening of muscle fibers and the densification of the cellular network (Fig. 1 a), leading to the formation of muscle tissue that is more mechanically adaptive 4 . This process is dynamic and progressive; during this densification process, muscle strength may increase up to threefold. However, challenges remain in applying similar structural methodologies to synthetic polymers in order to improve their performance. Stimulation methods—including mechanical force, light, and solvent molecules—have been reported to regulate the structure and enhance the performance of materials 5 – 11 . Among these, solvent molecular stimulation has garnered significant attention due to its operational simplicity and design flexibility. However, the use of organic solvents such as acetone 12 and ethanol 13 presents challenges, including toxicity, flammability, and limitations in performance improvement. In contrast, water, as a polar molecule, serves as an ecofriendly solvent and an essential component for the human biology. It plays a fundamental role in cellular metabolism by promoting the anabolic processes of muscle cells, thereby facilitating muscle growth and strength enhancement 14 . Inspired by mechanically enhanced structure of muscles, we developed a water-triggered supramolecular network composed of cellulose 15 – 21 and polymethyl methacrylate (PMMA) molecules, achieving breakthroughs in mechanical properties, low and high-temperature resistance, and moldability of the triggered polymer (noted as T-polymer). In its initial state, T-polymer features a stretchable supramolecular network characterized by flexibility and transparency, with a mechanical tensile strength of less than 3 MPa. Following water triggering, the stretchable network transforms into a dense cross-linked domain, accompanied by the formation of a stronger hydrogen bond (H-bond) network. This transformation is attributed to the hydrophobic-driven curling conformational behavior of PMMA molecules, leading to a substantial enhancement in mechanical properties of T-polymer, with tensile strength exceeding 60 MPa and Young's modulus reaching approximately 1.8 GPa—performance levels unattained by previously reported water-strengthened materials. T-polymer demonstrates water-dependent moldability, enabling customization and shaping into various designs. Moreover, this molding behavior is compatible with high-salinity seawater and textile wastewater, facilitating both the coloring and scalable design of T-polymer. The shaped products maintain their structural integrity without damage or melting under extreme conditions, including liquid nitrogen at -196°C and high temperatures up to 180°C. Although T-polymer possesses a plastic-like appearance, its mechanical performance, thermal resistance, low-temperature resistance, and recyclability surpass those of common plastics such as acrylonitrile-butadiene-styrene (ABS) and polylactic acid (PLA). Results Fabrication and performance of T-polymer A cellulose molecular network is initially constructed by disrupting the H-bonds within cellulose using 1-butyl-3-methylimidazolium chloride ([Bmim]Cl). Subsequently, a PMMA molecular network is introduced through in-situ polymerization of the methyl methacrylate monomer, resulting in the formation of stretchable cellulose-PMMA supramolecular network (left of Fig. 1 b). This unique supramolecular structure, in which the cellulose network serves as a molecular framework while PMMA functions as a water-responsive molecule to reinforce the structure, endows the T-polymer with triggering-enhanced characteristics resembling that of human muscle. During the water triggering of T-polymer, the hydrophobic nature of PMMA molecules causes water to promote the aggregation of -COOCH 3 /-CH 3 groups, reducing their interfacial contact with the aqueous phase. This leads to the formation of numerous hydrophobic clusters, transitioning the stretchable supramolecular network of T-polymer into densified cross-linked domain (right of Fig. 1 b). Throughout this process, the cellulose network acts as a spatially confining framework, effectively suppressing excessive aggregation of PMMA chains. This confinement not only ensures dimensional stability but also prevents the supramolecular structural collapse (Supplementary Figs. 1, 2). Additionally, water molecules contribute to the establishment of a robust H-bond network within T-polymer, which synergistically interacts with the clustered domains to further enhance the supramolecular architecture. This interaction facilitates the transition of T-polymer from a "soft state" to a "rigid state" (Fig. 1 c), significantly improving its mechanical properties. As illustrated in Fig. 1 d, the mechanical tensile strength of T-polymer increases from 2.7 MPa to 61.7 MPa, representing an augmentation of over 22 times. A mere 0.96 g of T-polymer can support loads exceeding 16,000 times its own weight while maintaining full structural integrity; furthermore, the T-polymer is accompanied by a notable optical change, transitioning from a transparent state to a white state (Supplementary Fig. 3), akin to that of commercial plastics. In comparison to commercial plastics such as PMMA, PLA, and ABS (Fig. 1 e), T-polymer demonstrates overall superiority in mechanical properties, high-temperature resistance (close to 200°C), low-temperature resistance (-196°C), and shapeability. Mechanism of supramolecular networks reconstruction We conducted molecular dynamics (MD) simulations to elucidate the mechanisms underlying supramolecular structural evolution during water-triggering process. As demonstrated in Fig. 2 a, water molecule facilitates the interaction between cellulose (Cel) and PMMA molecules, leading to the formation of a denser network structure. This transformation enables T-polymer to transition from a soft state to a rigid, hard state (Fig. 2 b). In contrast to mechanical training that enhances muscle strength by thickening muscle fibers and densifying cellular network, T-polymer exhibits significant reconstruction of supramolecular configuration from stretchable network into a densified cross-linked domain after water triggering. As shown in Fig. 2 c, the cellulose and PMMA molecular chains within rigid T-polymer display a higher root-mean-square deviation (RMSD), with the conformational change amplitude of PMMA molecules increasing fourfold compared to that of cellulose molecules. This observation suggests that water molecules primarily induce conformational changes for PMMA molecules, that is attributed to the presence of hydrophobic -COOCH 3 and -CH 3 groups. As depicted in Fig. 2 d, the PMMA molecule shows a greater reduction in end-to-end distance than cellulose, indicating a tendency for spatially curled conformational behavior. This design enables the cellulose molecule within T-polymer to serve as a structural framework while the coiled PMMA molecule provide crosslinking reinforcement, thereby densifying the supramolecular network and resulting in a decrease in the solvent-accessible surface area (Fig. 2 e). Additionally, this water triggering increased the number of H-bonds in Cel-PMMA and Cel-Cel (Fig. 2 f), while also enhancing the intermolecular electrostatic energy and van der Waals energy (Fig. 2 g and h), which will undoubtedly endow T-polymer with excellent mechanical properties and high/low temperature resistance. Another surprise is that T-polymer demonstrates controllable water-shaping characteristics, which can be accomplished at room temperature without the need for additional heat sources or organic solvents. As shown in Fig. 2 i and Supplementary Video 1, a rectangular T-polymer wrapped around a glass rod can achieve its three-dimensional (3D) structural design through water triggering in just 15 s. Compared to the shaping behaviors that rely on organic solvents 12 , 22 , this water shapeability of T-polymer is safer, more ecofriendly, and scalable. Additionally, the shaping characteristics of T-polymer are not limited to everyday freshwater but can also be extended to seawater and other low-value water resources. Structural characteristic and performance In addition to MD simulations, several characterization techniques—including Raman spectroscopy, small-angle X-ray scattering (SAXS), X-ray photoelectron spectroscopy (XPS), and scanning electron microscopy (SEM)—were utilized to investigate the supramolecular structural evolution of T-polymers during the water triggering process. As illustrated in Fig. 3 a, T-polymer gradually transitions from a soft to a rigid state within 30 s of water triggering. This transition is accompanied by the formation of crosslinked domains and a densification of the cellulose and PMMA supramolecular network. As water triggering progressed (Fig. 3 b), the peaks at 600 cm⁻¹ (-C-COO-) and 814 cm⁻¹ (-C-O-CH₃) (attributed to the -COOCH₃ groups in PMMA) exhibited a gradual increase in intensity, indicating that these groups showed an aggregation behavior driven by hydrophobic interactions. This aggregation would lead to a transformation of the coiled conformation of PMMA molecular chains within T-polymer. Further 2D Raman analysis of T-polymer demonstrated that, as depicted in Fig. 3 c, the signal intensity of -COOCH₃ groups was significantly stronger after water triggering compared to before, indicating the formation of a dense network structure in T-polymer. Observation of the SAXS curves revealed sharper and more intense characteristic diffraction peaks for T-polymer (Fig. 3 d), along with larger scattering rings (insets of Fig. 3 d). According to Bragg's law, these features indicate closer molecular packing and reduced interdomain distances within T-polymer. Moreover, X-ray diffraction (XRD) analysis showed that the intensity of diffraction peaks progressively enhanced with extended water triggering time (Supplementary Fig. 4), suggesting improved structural ordering and a dense supramolecular network. Comparative examination through SEM (Fig. 3 e) and 3D surface microtopography images (Supplementary Fig. 5) of T-polymers indicated that after 2 h of water triggering, T-polymer exhibited prominent clustered structural features, which arose from the water-induced coiling and clustering of supramolecular network. Simultaneously, XPS analysis indicated a systematic shift toward lower binding energies for both the O–C = O/C–O–C and C–H peaks in the C1s spectrum, as well as for the O–C = O and C–O–H/C–O–C peaks in the O1s spectrum during water triggering process (Supplementary Fig. 6). This reduction in binding energy signifies the formation of an enhanced intermolecular H-bonding network following water triggering. These H-bonds serve as dynamic cross-linking points, strengthening interchain interactions and endowing T-polymer with robust mechanical properties and structural stability. As shown in Fig. 3 f-h and Supplementary Figs. 7 and 8, T-polymer triggered by water exhibited highly mechanical performance, with tensile strength and Young’s modulus reaching 57 MPa and 1.5 GPa, respectively. Notably, the robust T-polymer, weighing only 5.3 g, easily supports a 1 kg load without observable deformation (Fig. 3 h). Mechanical properties of T-polymer Comparing T-polymer with rigid commercial plastics highlights the advantages of water triggering in enhancing its mechanical properties. As shown in Fig. 4 a, under the same nanoindentation load, T-polymer exhibits a smallest nanoindentation depth compared to plastics such as ABS, PMMA, and PLA. Due to the densely supramolecular configuration, T-polymer presents superior indentation hardness of 0.598 GPa (Fig. 4 b), stiffness of 3.23 µN/nm (Supplementary Fig. 9a), and modulus of 9.59 GPa (Supplementary Fig. 9b). In terms of macroscopic mechanical properties, T-polymer also demonstrates attractive mechanical properties (Fig. 4 c), with a tensile strength and Young’s modulus of 61.7 MPa and 1.8 GPa (Fig. 4 d), respectively, which outperforms plastics such as ABS, PMMA, and PLA. When compared with reported biobased plastics 23 – 32 (Fig. 4 e) and a wider range of commonly used petrochemical plastics 24 (Fig. 4 f), T-polymer still exhibits advantages in terms of tensile strength and Young’s modulus. Fatigue resistance, which refers to a material's intrinsic ability to resist crack propagation under cyclic mechanical loading, is crucial for ensuring long-term structural reliability 33 – 36 . Conventional plastics frequently experience mechanical degradation when subjected to cyclic loading, resulting in crack propagation and eventual structural failure. In contrast, T-polymer preserves its structural integrity after 50 tensile cycles at a constant stress of 30 MPa (approximately 50% of its static tensile strength) and exhibits highly reproducible loading–unloading curves (Supplementary Fig. 10). This behavior indicates exceptional fatigue resistance and underscores T-polymer's potential for long-term durability. Flexural properties and impact resistance are essential performance metrics for materials in practical applications. Notably, T-polymer exhibits remarkable bending resistance (Fig. 4 g), boasting a flexural strength of 97 MPa and a flexural modulus of 4.085 GPa (Fig. 4 h and i), which highlights its superior ability to resist deformation compared to various commercial plastics (Supplementary Fig. 11). Furthermore, T-polymer retains its structural integrity even when subjected to bending beyond 180° (Fig. 4 j), a performance capability that many conventional plastics cannot achieve, such as ABS, PMMA, and PLA. Additionally, T-polymer exhibits exceptional impact resistance. In a drop-weight impact test, a 256 g steel ball is released from a height of 3 m. While reference plastics such as PMMA, PLA, and ABS suffer severely broken, T-polymer remains intact and demonstrates attractive instantaneous breakage resistance (Supplementary Fig. 12), with a specific fracture energy of 5.1 kJ·m⁻¹·(g·cm⁻³)⁻¹ (Fig. 4 k). In puncture resistance testing using a 60° conical probe, T-polymer achieves a specific puncture energy absorption of 1.117 kJ·m⁻¹·(g·cm⁻³)⁻¹—more than seven times that of PMMA, over six times that of PLA, and twice that of ABS (Fig. 4 k). Even after being subjected to a puncture test from a height of 1.2 m, T-polymer also retains its structural integrity with only minor indentation (Supplementary Fig. 13). High and low temperature resistance characteristics Beyond the exceptional mechanical properties, T-polymer demonstrates impressive resistance to extreme environmental conditions, providing a broad operational range and a robust foundation for practical applications. We utilize dynamic mechanical analysis (DMA) to examine the thermomechanical behavior of T-polymer. As illustrated in Fig. 5 a, the storage modulus (G′) of commercial plastics, such as ABS, diminishes to nearly zero at temperatures below 115°C. In contrast, T-polymer retains a higher G′ and exhibits detectable elastic responses even at 180°C. Simultaneously, the loss modulus (G″) of T-polymer remains consistently low (Supplementary Fig. 14a), exhibiting no prominent peak and consistently falling below the values of G′. These indicate that T-polymer predominantly showcases elastic solid-like characteristics under high-temperature environment. As depicted in Supplementary Fig. 14b, while commercial plastics, including ABS, display a tan δ greater than 1, T-polymer consistently maintains a tan δ below 1, further confirming that its deformation is primarily elastic in the solid state. Except for T-polymer, all petrochemical plastics exhibit varying degrees of flow deformation, ultimately leading to structural failure (Supplementary Fig. 14c). Thermogravimetry (TG) tests reveal that T-polymer has a notably high onset decomposition temperature of 290°C, significantly surpassing that of ABS, PMMA, and PLA plastics (Fig. 5 b). This exceptional thermal stability is attributed to its densely structural domains. To assess the impact of high-temperature exposure on mechanical behaviors, we conducted tensile tests on polymers that were subjected to treatment at 180°C for 1 h. As illustrated in Fig. 5 c and d, T-polymer exhibits higher tensile strength and Young’s modulus compared to petrochemical plastics. Remarkably, even after being exposed to 180°C for 3 h, T-polymer retained its structural integrity, while the compared petrochemical plastics exhibited significant deformation and damage (Fig. 5 e), highlighting a sharp contrast in performance. In addition to its high-temperature resistance, T-polymer also demonstrates remarkable cryogenic stability. As illustrated in Fig. 5 f, even after immersion in liquid nitrogen (–196°C) for 3 min, T-polymer maintains its toughness and foldability with high tensile strength of over 40 MPa (Fig. 5 g), whereas all ABS, PMMA, and PLA samples exhibited significant bending failure. This may contribute to the application of T-polymer as a lightweight, cold-resistant material in aerospace and arctic exploration equipment. To elucidate the mechanisms behind its low-temperature resistance, we systematically evaluated several potential contributing factors. As shown in Supplementary Figs. 15 and 16, the cryogenic resistance of T-polymer arises from the synergistic effects of multiple factors. The formation of cross-linked domains and densified supramolecular networks plays a critical role in minimizing energy dissipation, thereby ensuring structural integrity under cryogenic conditions. Encouragingly, T-polymer exhibits exceptional dimensional stability under humid conditions. After 15 d of exposure at either 50% or 90% relative humidity (RH), its dimensions remain essentially unchanged; even after 30 d, the size retention rate exceeds 95%. In addition to its outstanding performances in extreme environments, T-polymer demonstrates remarkable solvent resistance. As illustrated in Supplementary Fig. 17, T-polymer retains its original shape and stiffness after 30 d of immersion in various acidic, alkaline, saline, and organic solvents. Application, biocompatibility and economic feasibility of T-polymer While polymer chains can be reprocessed at elevated temperatures, this approach suffers from notable limitations. The considerable energy consumption associated with thermal processing, coupled with undesirable side reactions such as oxidative degradation and chain scission, often results in a marked decline in the performance of thermoplastics after several recycling cycles 37 – 40 . In contrast to traditional petrochemical plastic processing, T-polymer can be easily shaped into various forms through water-shaping at room temperature (Fig. 6 a, Supplementary Fig. 18a). Additionally, during the initial stages of gel formation, its fluidity can be exploited for injection molding (middle of Fig. 6 a, Supplementary Fig. 18b). These versatile processing methods significantly enhance the applicability and scalability of T-polymer. Leveraging its exceptional water-triggered plasticity, we developed a functional container designed to meet practical needs (Fig. 6 a, right). This container demonstrates impressive water stability and leakage resistance. Comparative contact angle measurements indicate a substantially larger contact angle for T-polymer (Supplementary Fig. 19), which likely accounts for its superior hydrostability. As evidenced in Supplementary Fig. 20, various structural T-polymers produced using this aqueous shaping technique can support weights vastly exceeding their own, ranging from hundreds to tens of thousands of times their weight. For example, three S-shaped T-polymer components, with a combined mass of only 0.68 g, successfully support an 80 kg adult (Supplementary Fig. 20c). This remarkable load-bearing capacity provides a compelling basis for real-world applications. To explore the potential of T-polymer in biological contexts, we evaluated its biocompatibility. Cytotoxicity assays indicated excellent biocompatibility, with relative cell viability exceeding 100%, alongside evidence of a pro-proliferative effect (Fig. 6 b, left). Live staining confocal microscopy further confirmed the outstanding biocompatibility of T-polymer, revealing almost no detectable dead cells within the culture system (Fig. 6 b, right). These findings substantiate its potential applications in biologically relevant settings. In terms of sustainability, T-polymer exhibits promising recyclability. Its recycling process capitalizes on the reusability of [Bmim]Cl and DMSO used during production, thereby further reducing manufacturing costs. As illustrated in Fig. 6 c, the procedure involves two key steps: first, T-polymer particles are mixed with recycled [Bmim]Cl to create a soft-state polymer; second, structural densification and cross-linked domain formation are induced via water triggering to regenerate T-polymer. The recycled T-polymer maintains excellent mechanical properties, with a tensile strength of 49 MPa and an elastic modulus of 1.6 GPa (Fig. 6 d), comparable to those of the original material, thus confirming the repeatability and practicality of this recycling approach. A techno-economic analysis indicates that the production cost of T-polymer is slightly higher than that of bioplastic PLA (Fig. 6 e, Supplementary Tables 1 and 2). This cost advantage primarily arises from the economic viability of lignocellulosic feedstocks and the reusability of [Bmim]Cl and DMSO. Furthermore, the process demonstrates low energy consumption, with electricity comprising only 2.68% of the total production cost, enhancing its economic and environmental appeal. Although the production cost of T-polymer is slightly higher at $ 2,946.36 per ton, its combination of high mechanical strength, exceptional resistance to extreme environments, biocompatibility, and energy-efficient processability positions it favorably for advanced applications within the high-performance plastics market. Moreover, the water-triggering method we propose is applicable to various water quality environments. As illustrated in Fig. 7 a, high-salinity seawater, sludge water containing suspended solids, and textile wastewater with dyes can all effectively mechanically reinforce T-polymers, endowing them with shapable properties and attractive mechanical performances. Furthermore, utilizing textile wastewater facilitates the arbitrary and on-demand design of coloration for T-polymer. Compared to the mechanical triggering from tap-water, T-polymers triggered in seawater, sludge water, and textile wastewater also demonstrate excellent mechanical tensile performance (Fig. 7 b), with tensile strength and Young's modulus exceeding 50 MPa (Fig. 7 c) and 1.5 GPa (Fig. 7 d), respectively. Even in three-point flexural aspect, these T-polymers exhibit high mechanical performance characteristics (Fig. 7 e), with flexural strength and modulus exceeding 70 MPa (Fig. 7 f) and 3.5 GPa (Fig. 7 g), respectively. This universality contributes positively to efficient resource utilization and simplification of water resource acquisition, thereby providing a new material foundation for localized, low-consumption exploitation of various water resources. Discussion In this study, we introduce a water-triggering strategy designed to enhance the properties of polymers. This approach leverages the stimulus responsiveness of a polymer composed of a cellulose and PMMA supramolecular network to water, facilitating structural densification and performance improvement through a straightforward water triggering process. Notably, the enhancement in mechanical performance is achieved without compromising processability or environmental tolerance. The water-triggered polymer exhibits a tensile strength of 61.7 MPa and a Young’s modulus of 1.8 GPa, while demonstrating excellent temperature tolerance by maintaining structural integrity and mechanical robustness even after exposure to temperatures as high as 180°C or as low as -196°C. Moreover, this polymer can be shaped at room temperature through water triggering, in stark contrast to the energy-intensive thermal processing typically required for conventional polymers. Additionally, water-triggering polymer exhibits outstanding biocompatibility, supporting its potential applications in the biological field. From an economic standpoint, the production cost of this polymer is approximately $ 2,946.36 per ton, which provides a competitive advantage within the broader polymer market. Additionally, the polymer is also not highly selective regarding water quality, demonstrating its versatility across various water environments. The multifaceted advantages of polymer in terms of performance, sustainability, and processability position it as a promising candidate for next-generation sustainable high-performance polymers. This water triggering strategy paves the way for designing polymers that combine high performance with environmentally friendly manufacturing processes. Declarations Competing interests The authors declare no competing interests. Author contributions D.Z. and H.Y. supervised the project and designed the experiments. C.L. carried out most of the experiments. G.J., and M.W. participated in the experiments and contributed to the analysis of mechanical and thermal performances. G.C. provided valuable contributions to the cytotoxicity assessment and techno-economic analysis. C.L. wrote the paper. D.Z., H.Y., and G.C. discussed the results and designed the mechanism. D.Z., H.Y., and G.C. collectively reviewed the paper. All authors discussed the results and commented on the manuscript. Acknowledgments D.Z. acknowledges the support by the National Key Research and Development Program of China (No. 2023YFD2200504), the National Natural Science Foundation of China (No. 32371823) and the Liaoning Province Xingliao Talents Leading Talent Program (Grant No: XLYC2402043). Data availability The data supporting the findings of this work are available within the article and its supplementary files. All data are available from the corresponding author upon request. References Zhao S et al (2025) Directional vaporization-driven alignment in printable muscle-mimetic anisotropic protein materials. 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Supplementary Files VideoS1Mechanicalreinforcementandprogrammablebehaviorofwatertriggeredsupramolecularpolymers.mp4 Supplementary Video 1 SupplementaryInformation.docx Supplementary Information Cite Share Download PDF Status: Under Review Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. Our growing team is made up of researchers and industry professionals working together to solve the most critical problems facing scientific publishing. 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Zhao","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAA9ElEQVRIiWNgGAWjYDCCA0CcACLZG2BCCcRq4QGxGAyI1AImJRKI1MJ3/Izhgwd/7sjzSz5/Js1T84eBnz3HgOHnDtxaJM/kGBsk8DwznDk7x0ya55gBg2TPGwPG3jO4tRgcyN0mkSBxmHHD7Rw2ad4GAwaDGzkGzIxteLScf7v9R4LBYfsNN48/A2uxJ6jlRu42hoSEw4kbbjCYQWyRIKBF8sb7zxIJBw4nz+zJMbacc8yYR+LMs4KDvXi08J1PS/z4489h23724w9vvKmRk+NvT9744CceLciARQJI8IBYB4jTwMDA/IFYlaNgFIyCUTCyAACM3VZK1BI0HwAAAABJRU5ErkJggg==","orcid":"https://orcid.org/0000-0003-2813-7263","institution":"Northeast Forestry University; Shenyang University of Chemical Technology","correspondingAuthor":true,"prefix":"","firstName":"Dawei","middleName":"","lastName":"Zhao","suffix":""},{"id":566969587,"identity":"c23a2880-7c6d-4145-84dd-a18625ef9390","order_by":1,"name":"Changhong Lin","email":"","orcid":"","institution":"Shenyang University of Chemical 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13:15:33","extension":"xml","order_by":18,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":91585,"visible":true,"origin":"","legend":"","description":"","filename":"NCOMMS250992590structuring.xml","url":"https://assets-eu.researchsquare.com/files/rs-8305182/v1/dd53b2643970418fb7d63901.xml"},{"id":99793354,"identity":"85cd597f-99f4-4e2d-9e67-74a2f5db38f1","added_by":"auto","created_at":"2026-01-08 13:31:27","extension":"html","order_by":19,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":101381,"visible":true,"origin":"","legend":"","description":"","filename":"earlyproof.html","url":"https://assets-eu.researchsquare.com/files/rs-8305182/v1/cd7f52473cc86e570bae1665.html"},{"id":99572585,"identity":"19bfff32-cb9a-4d98-a973-c50090eef297","added_by":"auto","created_at":"2026-01-06 03:07:28","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":3322873,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eBionic design and preparation of T-polymer. a\u003c/strong\u003e Mechanical training to enhance the performance of human muscle. \u003cstrong\u003eb \u003c/strong\u003eSupramolecular network reconstruction during the water triggering process. Each element of schematic diagram was conceived by the authors of this work and drawn using Adobe Photoshop CC 2019 and 3ds Max 2018 software. \u003cstrong\u003ec\u003c/strong\u003e Optical images displaying the transition of T-polymer from a soft to a rigid state after triggered by water molecules. \u003cstrong\u003ed\u003c/strong\u003e Improvement of the tensile strength of T-polymer.\u003cstrong\u003e e\u003c/strong\u003e Radar plot of T-polymer and commercial plastics (PMMA, PLA, ABS).\u003c/p\u003e","description":"","filename":"floatimage1.png","url":"https://assets-eu.researchsquare.com/files/rs-8305182/v1/7cf952bf2423f2c49c451b0b.png"},{"id":99572606,"identity":"ecdd7cdc-623b-4e0a-91f5-06718ca2122e","added_by":"auto","created_at":"2026-01-06 03:07:29","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":2253129,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eSupramolecular regulation mechanism of T-polymer during water triggering process.\u003c/strong\u003e \u003cstrong\u003ea\u003c/strong\u003e MD snapshots of T-polymer before and after water triggering. \u003cstrong\u003eb\u003c/strong\u003e Optical images of T-polymer from soft state into rigid state. \u003cstrong\u003ec\u003c/strong\u003e Investigating the RMSD values of cellulose and PMMA molecules during different states. \u003cstrong\u003ed\u003c/strong\u003e Comparation of end-to-end distance of cellulose and PMMA molecules during different states. \u003cstrong\u003ee\u003c/strong\u003e Solvent-accessible surface area of cellulose and PMMA molecules during different states. \u003cstrong\u003ef \u003c/strong\u003eNumber of H-bonds between cellulose and PAAM (Cel-PMMA), along with those involving other components, simulated by MD. \u003cstrong\u003eg\u003c/strong\u003e Electrostatic energy of Cel-PMMA and other combinations simulated by MD. \u003cstrong\u003eh\u003c/strong\u003e Van der Waals energy of Cel-PMMA and other combinations simulated by MD. \u003cstrong\u003ei \u003c/strong\u003eOptical images of T-polymer showing the unique water-shaping capability.\u003c/p\u003e","description":"","filename":"floatimage2.png","url":"https://assets-eu.researchsquare.com/files/rs-8305182/v1/59c751f91864523622b31996.png"},{"id":99572586,"identity":"540c4a98-6a45-4748-8cd7-92506a12a098","added_by":"auto","created_at":"2026-01-06 03:07:28","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":3318079,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eStructural and interaction analyses of T-polymer.\u003c/strong\u003e \u003cstrong\u003ea\u003c/strong\u003eOptical images of T-polymers during water triggering process. \u003cstrong\u003eb\u003c/strong\u003e Raman curves of T-polymers during water triggering process. \u003cstrong\u003ec\u003c/strong\u003e 2D Raman mappings of T-polymer (corresponding to -COOCH₃ groups) before and after water triggering. \u003cstrong\u003ed\u003c/strong\u003e SAXS curves and 2D images of T-polymers with different states. \u003cstrong\u003ee\u003c/strong\u003e SEM images of T-polymers. \u003cstrong\u003ef \u003c/strong\u003eStress-strain curves of T-polymers during water triggering process. \u003cstrong\u003eg\u003c/strong\u003e Comparison of Young’s modulus of T-polymers with different water triggering time. Values in \u003cstrong\u003eg\u003c/strong\u003e represent their means ± SDs from \u003cem\u003en\u003c/em\u003e = 5 independent samples. \u003cstrong\u003eh\u003c/strong\u003e Load-bearing image of T-polymer after 2 h of water triggering.\u003c/p\u003e","description":"","filename":"floatimage3.png","url":"https://assets-eu.researchsquare.com/files/rs-8305182/v1/02447860c27101720d3628dc.png"},{"id":99793107,"identity":"9c86c8be-ea2a-4463-9451-a4d788437805","added_by":"auto","created_at":"2026-01-08 13:31:02","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":904395,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eExcellent mechanical performance of T-polymer.\u003c/strong\u003e \u003cstrong\u003ea\u003c/strong\u003e Load–displacement curves for static nanoindentation tests of T-polymer and commercial plastics. \u003cstrong\u003eb\u003c/strong\u003eComparison of hardness of ABS, PMMA, PLA, and T-polymer. \u003cstrong\u003ec\u003c/strong\u003e Tensile stress-strain curves of ABS, PMMA, PLA, and T-polymer.All samples have thickness of 1.00 ± 0.01mm. \u003cstrong\u003ed\u003c/strong\u003e Comparison of tensile strength and modulus of ABS, PMMA, PLA, and T-polymer. \u003cstrong\u003ee\u003c/strong\u003e Investigating the tensile strength between T-polymer and previously reported bioplastics. \u003cstrong\u003ef\u003c/strong\u003eInvestigating the tensile strength and modulus between T-polymer and commercial plastics. \u003cstrong\u003eg\u003c/strong\u003e Flexural strength-strain curves of ABS, PMMA, PLA, and T-polymer. All samples have thickness of 1.00 ± 0.01mm. \u003cstrong\u003eh\u003c/strong\u003e Comparison of flexural strength of ABS, PMMA, PLA, and T-polymer. \u003cstrong\u003ei\u003c/strong\u003e Comparison of flexural modulus of ABS, PMMA, PLA, and T-polymer. \u003cstrong\u003ej\u003c/strong\u003e Digital images of ABS, PMMA, PLA, and T-polymer after 180° bending. \u003cstrong\u003ek\u003c/strong\u003e Comparison of breakage resistance and specific puncture energy absorption between ABS, PMMA, PLA, and T-polymer. Values in (\u003cstrong\u003eb\u003c/strong\u003e, \u003cstrong\u003ed\u003c/strong\u003e,\u003cstrong\u003e h\u003c/strong\u003e,\u003cstrong\u003e i\u003c/strong\u003eand \u003cstrong\u003ek\u003c/strong\u003e) represent their means ± SDs from \u003cem\u003en\u003c/em\u003e = 5 independent samples.\u003c/p\u003e","description":"","filename":"floatimage4.png","url":"https://assets-eu.researchsquare.com/files/rs-8305182/v1/7b90d4d58b1ec3f5a26258ca.png"},{"id":99792094,"identity":"c8c51688-bda5-4337-be78-8e66883a676e","added_by":"auto","created_at":"2026-01-08 13:14:33","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":1407921,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eT-polymer's resistance to extreme temperatures.\u003c/strong\u003e \u003cstrong\u003ea\u003c/strong\u003e Comparison of the G′ between ABS, PMMA, PLA, and T-polymer. These curves are obtained through DMA testing. \u003cstrong\u003eb\u003c/strong\u003e TG curves of ABS, PMMA, PLA, and T-polymer. \u003cstrong\u003ec\u003c/strong\u003e Tensile stress-strain curves of ABS, PMMA, PLA, and T-polymer after being subjected to 180 ℃ heat treatment for 1 h. All samples have thickness of 1.00 ± 0.01mm. \u003cstrong\u003ed\u003c/strong\u003e Comparison of Young’s modulus of ABS, PMMA, PLA, and T-polymer after being subjected to 180 ℃ heat treatment for 1 h. Values in \u003cstrong\u003ed\u003c/strong\u003e represent their means ± SDs from \u003cem\u003en\u003c/em\u003e = 5 independent samples. \u003cstrong\u003ee\u003c/strong\u003eOptical images from high-temperature resistance experiments conducted on T-polymer and several petrochemical plastics. All samples have thickness of 1.00 ± 0.01mm. \u003cstrong\u003ef\u003c/strong\u003e Digital images from low-temperature resistance experiments conducted on T-polymer and several petrochemical plastics. All samples have thickness of 1.00 ± 0.01mm. \u003cstrong\u003eg\u003c/strong\u003e Tensile stress-strain curve of T-polymer after being subjected to -196 ℃ for 3 min. All samples have thickness of 1.00 ± 0.01mm. \u003cstrong\u003eh\u003c/strong\u003eOptical images of the shape retention of T-polymer under different RH. \u003cstrong\u003ei\u003c/strong\u003eInvestigating of the size retention rate of T-polymer under different RH.\u003c/p\u003e","description":"","filename":"floatimage5.png","url":"https://assets-eu.researchsquare.com/files/rs-8305182/v1/5254552199348cb957e21efc.png"},{"id":99572590,"identity":"990ffe9e-2f01-4a15-800b-fcea775c8973","added_by":"auto","created_at":"2026-01-06 03:07:29","extension":"png","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":3257929,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eRecyclability, biodegradability, and economic feasibility of T-polymer.\u003c/strong\u003e \u003cstrong\u003ea\u003c/strong\u003e Optical images of T-polymer showing customizable shapeability. \u003cstrong\u003eb\u003c/strong\u003e Analysis of cytotoxicity of T-polymer on normal skin fibroblast (NHDF) cells. The left figure shows the relative cell survival rate, while the right figure presents the confocal live-cell staining images under different extraction solution concentrations. \u003cstrong\u003ec\u003c/strong\u003eInvestigating the recyclability of T-polymer. \u003cstrong\u003ed\u003c/strong\u003e Tensile strength and modulus of recycled T-polymer. Values in \u003cstrong\u003ed\u003c/strong\u003e represent their means ± SDs from \u003cem\u003en\u003c/em\u003e = 5 independent samples. \u003cstrong\u003ee\u003c/strong\u003e Comparison of production costs of T-polymer and commercial plastics including PP, ABS, PMMA, PA66, and PLA.\u003c/p\u003e","description":"","filename":"floatimage6.png","url":"https://assets-eu.researchsquare.com/files/rs-8305182/v1/b15a804dce987f715a51d021.png"},{"id":99572601,"identity":"eee2cf22-4005-4783-bab2-ac57a05f1185","added_by":"auto","created_at":"2026-01-06 03:07:29","extension":"png","order_by":7,"title":"Figure 7","display":"","copyAsset":false,"role":"figure","size":3372437,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003eScalable water triggering strategy for T-polymers.\u003c/strong\u003e \u003cstrong\u003ea\u003c/strong\u003e Demonstration of the scalability of T-polymers in various water environments. \u003cstrong\u003eb\u003c/strong\u003e Tensile stress-strain curves of T-polymers subjected to mechanical triggered in different water environments. All samples have a thickness of 1.00 ± 0.01mm. \u003cstrong\u003ec\u003c/strong\u003eComparison of tensile strength of T-polymer triggered in various water environments. \u003cstrong\u003ed\u003c/strong\u003e Comparison of Young’s modulus of T-polymers. \u003cstrong\u003ee\u003c/strong\u003e Flexural strength-strain curves of T-polymer triggered in various water environments. All samples have a thickness of 1.00 ± 0.01mm. \u003cstrong\u003ef\u003c/strong\u003e Comparison of flexural strength of T-polymer triggered in different water environments. \u003cstrong\u003eg\u003c/strong\u003eComparison of flexural modulus of T-polymers. Values in (\u003cstrong\u003ec\u003c/strong\u003e, \u003cstrong\u003ed\u003c/strong\u003e,\u003cstrong\u003ef\u003c/strong\u003e and \u003cstrong\u003eg\u003c/strong\u003e) represent their means ± SDs from \u003cem\u003en\u003c/em\u003e = 5 independent samples.\u003c/p\u003e","description":"","filename":"floatimage7.png","url":"https://assets-eu.researchsquare.com/files/rs-8305182/v1/db410274345d440f35f6e4b1.png"},{"id":99804236,"identity":"2c232f17-efcb-456a-9b11-39e56ac4eab0","added_by":"auto","created_at":"2026-01-08 14:12:40","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":18069738,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-8305182/v1/cfa0ad01-cdce-4b21-8ae1-48037612d642.pdf"},{"id":99791743,"identity":"b669682f-cc19-4f66-bab7-53a3fee4e8bb","added_by":"auto","created_at":"2026-01-08 13:09:37","extension":"mp4","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":5305479,"visible":true,"origin":"","legend":"Supplementary Video 1","description":"","filename":"VideoS1Mechanicalreinforcementandprogrammablebehaviorofwatertriggeredsupramolecularpolymers.mp4","url":"https://assets-eu.researchsquare.com/files/rs-8305182/v1/8b1e68c532f5b9e6f92322c1.mp4"},{"id":99791736,"identity":"97d1baa3-8bd8-4095-a20f-3e0b28b06486","added_by":"auto","created_at":"2026-01-08 13:09:36","extension":"docx","order_by":2,"title":"","display":"","copyAsset":false,"role":"supplement","size":7970851,"visible":true,"origin":"","legend":"Supplementary Information","description":"","filename":"SupplementaryInformation.docx","url":"https://assets-eu.researchsquare.com/files/rs-8305182/v1/4339ad172959929cc7d01fd6.docx"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.","formattedTitle":"Bioinspired supramolecular polymers with water-triggered dense domains: achieving mechanical robustness, programmability, and weather resistance","fulltext":[{"header":"Introduction","content":"\u003cp\u003eMuscle development directly influences an individual's strength and endurance\u003csup\u003e\u003cspan additionalcitationids=\"CR2\" citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR3\" class=\"CitationRef\"\u003e3\u003c/span\u003e\u003c/sup\u003e. Mechanical training can promote the thickening of muscle fibers and the densification of the cellular network (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ea), leading to the formation of muscle tissue that is more mechanically adaptive\u003csup\u003e\u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e4\u003c/span\u003e\u003c/sup\u003e. This process is dynamic and progressive; during this densification process, muscle strength may increase up to threefold. However, challenges remain in applying similar structural methodologies to synthetic polymers in order to improve their performance.\u003c/p\u003e \u003cp\u003eStimulation methods\u0026mdash;including mechanical force, light, and solvent molecules\u0026mdash;have been reported to regulate the structure and enhance the performance of materials\u003csup\u003e\u003cspan additionalcitationids=\"CR6 CR7 CR8 CR9 CR10\" citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e\u003c/sup\u003e. Among these, solvent molecular stimulation has garnered significant attention due to its operational simplicity and design flexibility. However, the use of organic solvents such as acetone\u003csup\u003e\u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e\u003c/sup\u003e and ethanol\u003csup\u003e\u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e13\u003c/span\u003e\u003c/sup\u003e presents challenges, including toxicity, flammability, and limitations in performance improvement. In contrast, water, as a polar molecule, serves as an ecofriendly solvent and an essential component for the human biology. It plays a fundamental role in cellular metabolism by promoting the anabolic processes of muscle cells, thereby facilitating muscle growth and strength enhancement\u003csup\u003e\u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003eInspired by mechanically enhanced structure of muscles, we developed a water-triggered supramolecular network composed of cellulose\u003csup\u003e\u003cspan additionalcitationids=\"CR16 CR17 CR18 CR19 CR20\" citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e\u003c/sup\u003e and polymethyl methacrylate (PMMA) molecules, achieving breakthroughs in mechanical properties, low and high-temperature resistance, and moldability of the triggered polymer (noted as T-polymer). In its initial state, T-polymer features a stretchable supramolecular network characterized by flexibility and transparency, with a mechanical tensile strength of less than 3 MPa. Following water triggering, the stretchable network transforms into a dense cross-linked domain, accompanied by the formation of a stronger hydrogen bond (H-bond) network. This transformation is attributed to the hydrophobic-driven curling conformational behavior of PMMA molecules, leading to a substantial enhancement in mechanical properties of T-polymer, with tensile strength exceeding 60 MPa and Young's modulus reaching approximately 1.8 GPa\u0026mdash;performance levels unattained by previously reported water-strengthened materials.\u003c/p\u003e \u003cp\u003eT-polymer demonstrates water-dependent moldability, enabling customization and shaping into various designs. Moreover, this molding behavior is compatible with high-salinity seawater and textile wastewater, facilitating both the coloring and scalable design of T-polymer. The shaped products maintain their structural integrity without damage or melting under extreme conditions, including liquid nitrogen at -196\u0026deg;C and high temperatures up to 180\u0026deg;C. Although T-polymer possesses a plastic-like appearance, its mechanical performance, thermal resistance, low-temperature resistance, and recyclability surpass those of common plastics such as acrylonitrile-butadiene-styrene (ABS) and polylactic acid (PLA).\u003c/p\u003e"},{"header":"Results","content":"\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e \u003ch2\u003eFabrication and performance of T-polymer\u003c/h2\u003e \u003cp\u003eA cellulose molecular network is initially constructed by disrupting the H-bonds within cellulose using 1-butyl-3-methylimidazolium chloride ([Bmim]Cl). Subsequently, a PMMA molecular network is introduced through in-situ polymerization of the methyl methacrylate monomer, resulting in the formation of stretchable cellulose-PMMA supramolecular network (left of Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003eb). This unique supramolecular structure, in which the cellulose network serves as a molecular framework while PMMA functions as a water-responsive molecule to reinforce the structure, endows the T-polymer with triggering-enhanced characteristics resembling that of human muscle.\u003c/p\u003e \u003cp\u003eDuring the water triggering of T-polymer, the hydrophobic nature of PMMA molecules causes water to promote the aggregation of -COOCH\u003csub\u003e3\u003c/sub\u003e/-CH\u003csub\u003e3\u003c/sub\u003e groups, reducing their interfacial contact with the aqueous phase. This leads to the formation of numerous hydrophobic clusters, transitioning the stretchable supramolecular network of T-polymer into densified cross-linked domain (right of Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003eb). Throughout this process, the cellulose network acts as a spatially confining framework, effectively suppressing excessive aggregation of PMMA chains. This confinement not only ensures dimensional stability but also prevents the supramolecular structural collapse (Supplementary Figs.\u0026nbsp;1, 2).\u003c/p\u003e \u003cp\u003eAdditionally, water molecules contribute to the establishment of a robust H-bond network within T-polymer, which synergistically interacts with the clustered domains to further enhance the supramolecular architecture. This interaction facilitates the transition of T-polymer from a \"soft state\" to a \"rigid state\" (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ec), significantly improving its mechanical properties. As illustrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ed, the mechanical tensile strength of T-polymer increases from 2.7 MPa to 61.7 MPa, representing an augmentation of over 22 times. A mere 0.96 g of T-polymer can support loads exceeding 16,000 times its own weight while maintaining full structural integrity; furthermore, the T-polymer is accompanied by a notable optical change, transitioning from a transparent state to a white state (Supplementary Fig.\u0026nbsp;3), akin to that of commercial plastics. In comparison to commercial plastics such as PMMA, PLA, and ABS (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ee), T-polymer demonstrates overall superiority in mechanical properties, high-temperature resistance (close to 200\u0026deg;C), low-temperature resistance (-196\u0026deg;C), and shapeability.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003c/div\u003e\n\u003ch3\u003eMechanism of supramolecular networks reconstruction\u003c/h3\u003e\n\u003cp\u003eWe conducted molecular dynamics (MD) simulations to elucidate the mechanisms underlying supramolecular structural evolution during water-triggering process. As demonstrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea, water molecule facilitates the interaction between cellulose (Cel) and PMMA molecules, leading to the formation of a denser network structure. This transformation enables T-polymer to transition from a soft state to a rigid, hard state (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eb). In contrast to mechanical training that enhances muscle strength by thickening muscle fibers and densifying cellular network, T-polymer exhibits significant reconstruction of supramolecular configuration from stretchable network into a densified cross-linked domain after water triggering.\u003c/p\u003e \u003cp\u003eAs shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ec, the cellulose and PMMA molecular chains within rigid T-polymer display a higher root-mean-square deviation (RMSD), with the conformational change amplitude of PMMA molecules increasing fourfold compared to that of cellulose molecules. This observation suggests that water molecules primarily induce conformational changes for PMMA molecules, that is attributed to the presence of hydrophobic -COOCH\u003csub\u003e3\u003c/sub\u003e and -CH\u003csub\u003e3\u003c/sub\u003e groups. As depicted in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ed, the PMMA molecule shows a greater reduction in end-to-end distance than cellulose, indicating a tendency for spatially curled conformational behavior. This design enables the cellulose molecule within T-polymer to serve as a structural framework while the coiled PMMA molecule provide crosslinking reinforcement, thereby densifying the supramolecular network and resulting in a decrease in the solvent-accessible surface area (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ee).\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eAdditionally, this water triggering increased the number of H-bonds in Cel-PMMA and Cel-Cel (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ef), while also enhancing the intermolecular electrostatic energy and van der Waals energy (Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eg and h), which will undoubtedly endow T-polymer with excellent mechanical properties and high/low temperature resistance. Another surprise is that T-polymer demonstrates controllable water-shaping characteristics, which can be accomplished at room temperature without the need for additional heat sources or organic solvents. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ei and Supplementary Video 1, a rectangular T-polymer wrapped around a glass rod can achieve its three-dimensional (3D) structural design through water triggering in just 15 s. Compared to the shaping behaviors that rely on organic solvents\u003csup\u003e\u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e,\u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e22\u003c/span\u003e\u003c/sup\u003e, this water shapeability of T-polymer is safer, more ecofriendly, and scalable. Additionally, the shaping characteristics of T-polymer are not limited to everyday freshwater but can also be extended to seawater and other low-value water resources.\u003c/p\u003e\n\u003ch3\u003eStructural characteristic and performance\u003c/h3\u003e\n\u003cp\u003eIn addition to MD simulations, several characterization techniques\u0026mdash;including Raman spectroscopy, small-angle X-ray scattering (SAXS), X-ray photoelectron spectroscopy (XPS), and scanning electron microscopy (SEM)\u0026mdash;were utilized to investigate the supramolecular structural evolution of T-polymers during the water triggering process. As illustrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ea, T-polymer gradually transitions from a soft to a rigid state within 30 s of water triggering. This transition is accompanied by the formation of crosslinked domains and a densification of the cellulose and PMMA supramolecular network.\u003c/p\u003e \u003cp\u003eAs water triggering progressed (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eb), the peaks at 600 cm⁻\u0026sup1; (-C-COO-) and 814 cm⁻\u0026sup1; (-C-O-CH₃) (attributed to the -COOCH₃ groups in PMMA) exhibited a gradual increase in intensity, indicating that these groups showed an aggregation behavior driven by hydrophobic interactions. This aggregation would lead to a transformation of the coiled conformation of PMMA molecular chains within T-polymer. Further 2D Raman analysis of T-polymer demonstrated that, as depicted in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ec, the signal intensity of -COOCH₃ groups was significantly stronger after water triggering compared to before, indicating the formation of a dense network structure in T-polymer. Observation of the SAXS curves revealed sharper and more intense characteristic diffraction peaks for T-polymer (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ed), along with larger scattering rings (insets of Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ed). According to Bragg's law, these features indicate closer molecular packing and reduced interdomain distances within T-polymer. Moreover, X-ray diffraction (XRD) analysis showed that the intensity of diffraction peaks progressively enhanced with extended water triggering time (Supplementary Fig.\u0026nbsp;4), suggesting improved structural ordering and a dense supramolecular network. Comparative examination through SEM (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ee) and 3D surface microtopography images (Supplementary Fig.\u0026nbsp;5) of T-polymers indicated that after 2 h of water triggering, T-polymer exhibited prominent clustered structural features, which arose from the water-induced coiling and clustering of supramolecular network.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eSimultaneously, XPS analysis indicated a systematic shift toward lower binding energies for both the O\u0026ndash;C\u0026thinsp;=\u0026thinsp;O/C\u0026ndash;O\u0026ndash;C and C\u0026ndash;H peaks in the C1s spectrum, as well as for the O\u0026ndash;C\u0026thinsp;=\u0026thinsp;O and C\u0026ndash;O\u0026ndash;H/C\u0026ndash;O\u0026ndash;C peaks in the O1s spectrum during water triggering process (Supplementary Fig.\u0026nbsp;6). This reduction in binding energy signifies the formation of an enhanced intermolecular H-bonding network following water triggering. These H-bonds serve as dynamic cross-linking points, strengthening interchain interactions and endowing T-polymer with robust mechanical properties and structural stability. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ef-h and Supplementary Figs.\u0026nbsp;7 and 8, T-polymer triggered by water exhibited highly mechanical performance, with tensile strength and Young\u0026rsquo;s modulus reaching 57 MPa and 1.5 GPa, respectively. Notably, the robust T-polymer, weighing only 5.3 g, easily supports a 1 kg load without observable deformation (Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eh).\u003c/p\u003e\n\u003ch3\u003eMechanical properties of T-polymer\u003c/h3\u003e\n\u003cp\u003eComparing T-polymer with rigid commercial plastics highlights the advantages of water triggering in enhancing its mechanical properties. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ea, under the same nanoindentation load, T-polymer exhibits a smallest nanoindentation depth compared to plastics such as ABS, PMMA, and PLA. Due to the densely supramolecular configuration, T-polymer presents superior indentation hardness of 0.598 GPa (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eb), stiffness of 3.23 \u0026micro;N/nm (Supplementary Fig.\u0026nbsp;9a), and modulus of 9.59 GPa (Supplementary Fig.\u0026nbsp;9b). In terms of macroscopic mechanical properties, T-polymer also demonstrates attractive mechanical properties (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ec), with a tensile strength and Young\u0026rsquo;s modulus of 61.7 MPa and 1.8 GPa (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ed), respectively, which outperforms plastics such as ABS, PMMA, and PLA. When compared with reported biobased plastics\u003csup\u003e\u003cspan additionalcitationids=\"CR24 CR25 CR26 CR27 CR28 CR29 CR30 CR31\" citationid=\"CR23\" class=\"CitationRef\"\u003e23\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e\u003c/sup\u003e (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ee) and a wider range of commonly used petrochemical plastics\u003csup\u003e\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e\u003c/sup\u003e (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ef), T-polymer still exhibits advantages in terms of tensile strength and Young\u0026rsquo;s modulus.\u003c/p\u003e \u003cp\u003eFatigue resistance, which refers to a material's intrinsic ability to resist crack propagation under cyclic mechanical loading, is crucial for ensuring long-term structural reliability\u003csup\u003e\u003cspan additionalcitationids=\"CR34 CR35\" citationid=\"CR33\" class=\"CitationRef\"\u003e33\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e36\u003c/span\u003e\u003c/sup\u003e. Conventional plastics frequently experience mechanical degradation when subjected to cyclic loading, resulting in crack propagation and eventual structural failure. In contrast, T-polymer preserves its structural integrity after 50 tensile cycles at a constant stress of 30 MPa (approximately 50% of its static tensile strength) and exhibits highly reproducible loading\u0026ndash;unloading curves (Supplementary Fig.\u0026nbsp;10). This behavior indicates exceptional fatigue resistance and underscores T-polymer's potential for long-term durability.\u003c/p\u003e \u003cp\u003eFlexural properties and impact resistance are essential performance metrics for materials in practical applications. Notably, T-polymer exhibits remarkable bending resistance (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eg), boasting a flexural strength of 97 MPa and a flexural modulus of 4.085 GPa (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eh and i), which highlights its superior ability to resist deformation compared to various commercial plastics (Supplementary Fig.\u0026nbsp;11). Furthermore, T-polymer retains its structural integrity even when subjected to bending beyond 180\u0026deg; (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ej), a performance capability that many conventional plastics cannot achieve, such as ABS, PMMA, and PLA.\u003c/p\u003e \u003cp\u003eAdditionally, T-polymer exhibits exceptional impact resistance. In a drop-weight impact test, a 256 g steel ball is released from a height of 3 m. While reference plastics such as PMMA, PLA, and ABS suffer severely broken, T-polymer remains intact and demonstrates attractive instantaneous breakage resistance (Supplementary Fig.\u0026nbsp;12), with a specific fracture energy of 5.1 kJ\u0026middot;m⁻\u0026sup1;\u0026middot;(g\u0026middot;cm⁻\u0026sup3;)⁻\u0026sup1; (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ek). In puncture resistance testing using a 60\u0026deg; conical probe, T-polymer achieves a specific puncture energy absorption of 1.117 kJ\u0026middot;m⁻\u0026sup1;\u0026middot;(g\u0026middot;cm⁻\u0026sup3;)⁻\u0026sup1;\u0026mdash;more than seven times that of PMMA, over six times that of PLA, and twice that of ABS (Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ek). Even after being subjected to a puncture test from a height of 1.2 m, T-polymer also retains its structural integrity with only minor indentation (Supplementary Fig.\u0026nbsp;13).\u003c/p\u003e \u003cp\u003e \u003c/p\u003e\n\u003ch3\u003eHigh and low temperature resistance characteristics\u003c/h3\u003e\n\u003cp\u003eBeyond the exceptional mechanical properties, T-polymer demonstrates impressive resistance to extreme environmental conditions, providing a broad operational range and a robust foundation for practical applications. We utilize dynamic mechanical analysis (DMA) to examine the thermomechanical behavior of T-polymer. As illustrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ea, the storage modulus (G\u0026prime;) of commercial plastics, such as ABS, diminishes to nearly zero at temperatures below 115\u0026deg;C. In contrast, T-polymer retains a higher G\u0026prime; and exhibits detectable elastic responses even at 180\u0026deg;C. Simultaneously, the loss modulus (G\u0026Prime;) of T-polymer remains consistently low (Supplementary Fig.\u0026nbsp;14a), exhibiting no prominent peak and consistently falling below the values of G\u0026prime;. These indicate that T-polymer predominantly showcases elastic solid-like characteristics under high-temperature environment. As depicted in Supplementary Fig.\u0026nbsp;14b, while commercial plastics, including ABS, display a tan δ greater than 1, T-polymer consistently maintains a tan δ below 1, further confirming that its deformation is primarily elastic in the solid state. Except for T-polymer, all petrochemical plastics exhibit varying degrees of flow deformation, ultimately leading to structural failure (Supplementary Fig.\u0026nbsp;14c).\u003c/p\u003e \u003cp\u003eThermogravimetry (TG) tests reveal that T-polymer has a notably high onset decomposition temperature of 290\u0026deg;C, significantly surpassing that of ABS, PMMA, and PLA plastics (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eb). This exceptional thermal stability is attributed to its densely structural domains. To assess the impact of high-temperature exposure on mechanical behaviors, we conducted tensile tests on polymers that were subjected to treatment at 180\u0026deg;C for 1 h. As illustrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ec and d, T-polymer exhibits higher tensile strength and Young\u0026rsquo;s modulus compared to petrochemical plastics. Remarkably, even after being exposed to 180\u0026deg;C for 3 h, T-polymer retained its structural integrity, while the compared petrochemical plastics exhibited significant deformation and damage (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ee), highlighting a sharp contrast in performance.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eIn addition to its high-temperature resistance, T-polymer also demonstrates remarkable cryogenic stability. As illustrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ef, even after immersion in liquid nitrogen (\u0026ndash;196\u0026deg;C) for 3 min, T-polymer maintains its toughness and foldability with high tensile strength of over 40 MPa (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eg), whereas all ABS, PMMA, and PLA samples exhibited significant bending failure. This may contribute to the application of T-polymer as a lightweight, cold-resistant material in aerospace and arctic exploration equipment. To elucidate the mechanisms behind its low-temperature resistance, we systematically evaluated several potential contributing factors. As shown in Supplementary Figs.\u0026nbsp;15 and 16, the cryogenic resistance of T-polymer arises from the synergistic effects of multiple factors. The formation of cross-linked domains and densified supramolecular networks plays a critical role in minimizing energy dissipation, thereby ensuring structural integrity under cryogenic conditions.\u003c/p\u003e \u003cp\u003eEncouragingly, T-polymer exhibits exceptional dimensional stability under humid conditions. After 15 d of exposure at either 50% or 90% relative humidity (RH), its dimensions remain essentially unchanged; even after 30 d, the size retention rate exceeds 95%. In addition to its outstanding performances in extreme environments, T-polymer demonstrates remarkable solvent resistance. As illustrated in Supplementary Fig.\u0026nbsp;17, T-polymer retains its original shape and stiffness after 30 d of immersion in various acidic, alkaline, saline, and organic solvents.\u003c/p\u003e \u003cdiv id=\"Sec8\" class=\"Section2\"\u003e \u003ch2\u003eApplication, biocompatibility and economic feasibility of T-polymer\u003c/h2\u003e \u003cp\u003eWhile polymer chains can be reprocessed at elevated temperatures, this approach suffers from notable limitations. The considerable energy consumption associated with thermal processing, coupled with undesirable side reactions such as oxidative degradation and chain scission, often results in a marked decline in the performance of thermoplastics after several recycling cycles\u003csup\u003e\u003cspan additionalcitationids=\"CR38 CR39\" citationid=\"CR37\" class=\"CitationRef\"\u003e37\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR40\" class=\"CitationRef\"\u003e40\u003c/span\u003e\u003c/sup\u003e. In contrast to traditional petrochemical plastic processing, T-polymer can be easily shaped into various forms through water-shaping at room temperature (Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ea, Supplementary Fig.\u0026nbsp;18a). Additionally, during the initial stages of gel formation, its fluidity can be exploited for injection molding (middle of Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ea, Supplementary Fig.\u0026nbsp;18b). These versatile processing methods significantly enhance the applicability and scalability of T-polymer.\u003c/p\u003e \u003cp\u003eLeveraging its exceptional water-triggered plasticity, we developed a functional container designed to meet practical needs (Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ea, right). This container demonstrates impressive water stability and leakage resistance. Comparative contact angle measurements indicate a substantially larger contact angle for T-polymer (Supplementary Fig.\u0026nbsp;19), which likely accounts for its superior hydrostability. As evidenced in Supplementary Fig.\u0026nbsp;20, various structural T-polymers produced using this aqueous shaping technique can support weights vastly exceeding their own, ranging from hundreds to tens of thousands of times their weight. For example, three S-shaped T-polymer components, with a combined mass of only 0.68 g, successfully support an 80 kg adult (Supplementary Fig.\u0026nbsp;20c). This remarkable load-bearing capacity provides a compelling basis for real-world applications.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eTo explore the potential of T-polymer in biological contexts, we evaluated its biocompatibility. Cytotoxicity assays indicated excellent biocompatibility, with relative cell viability exceeding 100%, alongside evidence of a pro-proliferative effect (Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003eb, left). Live staining confocal microscopy further confirmed the outstanding biocompatibility of T-polymer, revealing almost no detectable dead cells within the culture system (Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003eb, right). These findings substantiate its potential applications in biologically relevant settings.\u003c/p\u003e \u003cp\u003eIn terms of sustainability, T-polymer exhibits promising recyclability. Its recycling process capitalizes on the reusability of [Bmim]Cl and DMSO used during production, thereby further reducing manufacturing costs. As illustrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ec, the procedure involves two key steps: first, T-polymer particles are mixed with recycled [Bmim]Cl to create a soft-state polymer; second, structural densification and cross-linked domain formation are induced via water triggering to regenerate T-polymer. The recycled T-polymer maintains excellent mechanical properties, with a tensile strength of 49 MPa and an elastic modulus of 1.6 GPa (Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ed), comparable to those of the original material, thus confirming the repeatability and practicality of this recycling approach.\u003c/p\u003e \u003cp\u003eA techno-economic analysis indicates that the production cost of T-polymer is slightly higher than that of bioplastic PLA (Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ee, Supplementary Tables\u0026nbsp;1 and 2). This cost advantage primarily arises from the economic viability of lignocellulosic feedstocks and the reusability of [Bmim]Cl and DMSO. Furthermore, the process demonstrates low energy consumption, with electricity comprising only 2.68% of the total production cost, enhancing its economic and environmental appeal. Although the production cost of T-polymer is slightly higher at \u003cspan\u003e$\u003c/span\u003e2,946.36 per ton, its combination of high mechanical strength, exceptional resistance to extreme environments, biocompatibility, and energy-efficient processability positions it favorably for advanced applications within the high-performance plastics market.\u003c/p\u003e \u003cp\u003eMoreover, the water-triggering method we propose is applicable to various water quality environments. As illustrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ea, high-salinity seawater, sludge water containing suspended solids, and textile wastewater with dyes can all effectively mechanically reinforce T-polymers, endowing them with shapable properties and attractive mechanical performances. Furthermore, utilizing textile wastewater facilitates the arbitrary and on-demand design of coloration for T-polymer.\u003c/p\u003e \u003cp\u003eCompared to the mechanical triggering from tap-water, T-polymers triggered in seawater, sludge water, and textile wastewater also demonstrate excellent mechanical tensile performance (Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003eb), with tensile strength and Young's modulus exceeding 50 MPa (Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ec) and 1.5 GPa (Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ed), respectively. Even in three-point flexural aspect, these T-polymers exhibit high mechanical performance characteristics (Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ee), with flexural strength and modulus exceeding 70 MPa (Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ef) and 3.5 GPa (Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003eg), respectively. This universality contributes positively to efficient resource utilization and simplification of water resource acquisition, thereby providing a new material foundation for localized, low-consumption exploitation of various water resources.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003c/div\u003e"},{"header":"Discussion","content":"\u003cp\u003eIn this study, we introduce a water-triggering strategy designed to enhance the properties of polymers. This approach leverages the stimulus responsiveness of a polymer composed of a cellulose and PMMA supramolecular network to water, facilitating structural densification and performance improvement through a straightforward water triggering process. Notably, the enhancement in mechanical performance is achieved without compromising processability or environmental tolerance. The water-triggered polymer exhibits a tensile strength of 61.7 MPa and a Young\u0026rsquo;s modulus of 1.8 GPa, while demonstrating excellent temperature tolerance by maintaining structural integrity and mechanical robustness even after exposure to temperatures as high as 180\u0026deg;C or as low as -196\u0026deg;C.\u003c/p\u003e \u003cp\u003eMoreover, this polymer can be shaped at room temperature through water triggering, in stark contrast to the energy-intensive thermal processing typically required for conventional polymers. Additionally, water-triggering polymer exhibits outstanding biocompatibility, supporting its potential applications in the biological field. From an economic standpoint, the production cost of this polymer is approximately \u003cspan\u003e$\u003c/span\u003e2,946.36 per ton, which provides a competitive advantage within the broader polymer market.\u003c/p\u003e \u003cp\u003eAdditionally, the polymer is also not highly selective regarding water quality, demonstrating its versatility across various water environments. The multifaceted advantages of polymer in terms of performance, sustainability, and processability position it as a promising candidate for next-generation sustainable high-performance polymers. This water triggering strategy paves the way for designing polymers that combine high performance with environmentally friendly manufacturing processes.\u003c/p\u003e"},{"header":"Declarations","content":"\u003ch2\u003eCompeting interests\u003c/h2\u003e \u003cp\u003eThe authors declare no competing interests.\u003c/p\u003e\u003ch2\u003eAuthor contributions\u003c/h2\u003e \u003cp\u003eD.Z. and H.Y. supervised the project and designed the experiments. C.L. carried out most of the experiments. G.J., and M.W. participated in the experiments and contributed to the analysis of mechanical and thermal performances. G.C. provided valuable contributions to the cytotoxicity assessment and techno-economic analysis. C.L. wrote the paper. D.Z., H.Y., and G.C. discussed the results and designed the mechanism. D.Z., H.Y., and G.C. collectively reviewed the paper. All authors discussed the results and commented on the manuscript.\u003c/p\u003e\u003ch2\u003eAcknowledgments\u003c/h2\u003e \u003cp\u003eD.Z. acknowledges the support by the National Key Research and Development Program of China (No. 2023YFD2200504), the National Natural Science Foundation of China (No. 32371823) and the Liaoning Province Xingliao Talents Leading Talent Program (Grant No: XLYC2402043).\u003c/p\u003e\u003ch2\u003eData availability\u003c/h2\u003e \u003cp\u003eThe data supporting the findings of this work are available within the article and its supplementary files. All data are available from the corresponding author upon request.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\u003cli\u003e\u003cspan\u003eZhao S et al (2025) Directional vaporization-driven alignment in printable muscle-mimetic anisotropic protein materials. 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Adv Funct Mater 34:2306882\u003c/span\u003e\u003c/li\u003e\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":true,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":false,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"nature-portfolio","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"","title":"Nature Portfolio","twitterHandle":"","acdcEnabled":false,"dfaEnabled":false,"editorialSystem":"ejp","reportingPortfolio":"","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"cellulose, water-triggering, supramolecular polymer, shapeability, weather resistance","lastPublishedDoi":"10.21203/rs.3.rs-8305182/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-8305182/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eHuman muscles enhance their mechanical strength through structural training for densification of cellular networks; however, challenges remain in incorporating this feature into synthetic materials. Here, we report a water-triggered supramolecular polymer composed of cellulose and polymethyl methacrylate that achieves over a 22-fold improvement in mechanical properties. During this bioinspired process, water molecules trigger the transition of a stretchable supramolecular network into a densified cross-linked domain. The resultant polymer exhibits a remarkable increase in tensile strength from 2.7 MPa to 61.7 MPa, and demonstrate a substantial flexural strength of 97 MPa, while maintaining impressive structural integrity across a temperature range of -196\u0026deg;C to 180\u0026deg;C. In addition, the polymers possess scalable water-shaping and reinforcement capability, even in seawater or textile wastewater, retaining 100% of their mechanical performance, which allows for customization into tailored geometric structures. Economic analysis and recycling assessment demonstrate that this polymer possesses successful scalability and considerable market. This study provides a biomimetic formulation for the fabrication of high-performance supramolecular polymers, broadening their applications across various fields.\u003c/p\u003e","manuscriptTitle":"Bioinspired supramolecular polymers with water-triggered dense domains: achieving mechanical robustness, programmability, and weather resistance","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2026-01-06 03:07:23","doi":"10.21203/rs.3.rs-8305182/v1","editorialEvents":[],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"nature-communications","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"NCOMMS","sideBox":"Learn more about [Nature Communications](http://www.nature.com/ncomms/)","snPcode":"","submissionUrl":"https://mts-ncomms.nature.com/","title":"Nature Communications","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"ejp","reportingPortfolio":"Nature Communications","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"083bd402-0942-4e86-aedc-d999d314c798","owner":[],"postedDate":"January 6th, 2026","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"under-review","subjectAreas":[{"id":60347252,"name":"Physical sciences/Materials science/Soft materials/Polymers"},{"id":60347253,"name":"Physical sciences/Materials science/Nanoscale materials/Structural properties"}],"tags":[],"updatedAt":"2026-04-18T09:01:01+00:00","versionOfRecord":[],"versionCreatedAt":"2026-01-06 03:07:23","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-8305182","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-8305182","identity":"rs-8305182","version":["v1"]},"buildId":"XKTyCvWXoU3ODBz1xrDgd","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}