Bioinspired nano-architecture for cellulose fibers with spider silk–like toughness

Cellulose fibers derived from renewable biomass exhibit exceptional tensile strength through molecular alignment and dense packing, yet their toughness remains limited, typically below 50 MJ m −3 . Drawing inspiration from the helical nanoarchitecture of cherry bark, we introduce a bioinspired nano-orientation strategy to fabricate regenerated cellulose fibers with a biaxially oriented structure via a scalable microfluidic spinning technique. Combining experimental characterization and molecular simulations, we demonstrate that this biaxial nano-architecture effectively redistributes stress and suppresses crack propagation during deformation, achieving a remarkable fracture strain of 41% alongside a tensile strength of 553 MPa. This synergy yields a toughness of 184 MJ m −3 , exhibiting highly competitive performance relative to most previously reported cellulose fibers and synthetic polymers, and achieving a mechanical performance on the same order of magnitude as natural spider silk. Moreover, this enhancement extends seamlessly from single fibers to woven fabrics, highlighting its potential for sustainable, high-performance materials in textiles, automotive components, and aerospace applications. Our findings illuminate a design for overcoming the intrinsic brittleness of cellulose fibers, advancing their applicability as eco-friendly structural materials.