Bioinspired Spindles using Peptide-DNA Nanotechnology

Abstract Cytoskeletal assemblies produce functionality through multiscale structural reconfiguration by exploiting a family of protein crosslinkers. Inspired by these principles, we designed an array of complementary peptide-DNA monomers able to form multistranded junctions with different geometries and stabilities and tested their effect on the structural organization of co-polymerized filament-forming peptides. In striking similarity to their biological counterparts, the peptide-DNA crosslinkers organized fibers into bundled architectures with base-pair tunable aspect ratios. Controlling solvent or temperature drove assembly through distinct pathways to form different structural and mechanical states exhibiting multiple levels of hierarchy from the same set of components. The thermal reversibility of DNA crosslinks drove structures to form, disassemble, and rebuild over multiple cycles. Sequential transitioning between bundles and fibers using orthogonal triggers enabled the dosed release of proteins to modulate catalytic reactions. This programmable peptide-DNA nanotechnology framework will pave the way towards the design of hierarchical materials with reconfigurable properties.