LAUSR

Synthetic hydrogels are unique tissue mimics but rarely reproduce the strain‐stiffening properties of native tissues. This mechanical mismatch impairs the performance of hydrogels in practical applications. Inspired by the crimped structure of collagenous tissues, a series of strain‐stiffening hydrogels composed of curved parallel fibers are developed. These fibers are constructed from a bundle of intertwisted nanofibrils composed of short alkyl side chain‐modified polymer chains. This hierarchical organization enables exquisitely cascaded deformation that facilitates soft‐to‐firm and resilience‐to‐viscoelasticity transitions, thus synergically mimicking the strain‐adaptive stiffening and damping behaviors of natural tissues. Together with structural evolution and a constitutive model, rationally tuning the tortuosity and flexibility of the curved fibers produces a diverse combination of strain‐stiffening properties and unprecedented penetration into the regions of several tissues. The crimped structure and the resultant stiffening properties constitute major improvements to nanofiber‐based scaffolds for use in collagenous tissue repair.