Natural-Wood-Inspired Ultrastrong Anisotropic Hybrid Hydrogels Targeting Artificial Tendons or Ligaments

Hydrogels are able to mimic the flexibility of biological tissues or skin, but they still cannot achieve satisfactory strength and toughness, greatly limiting their scope of application. Natural wood can offer inspiration for designing high-strength hydrogels attributed to its anisotropic structure. Herein, we propose an integrated strategy for efficient preparation of ultrastrong hydrogels using a salting-assisted prestretching treatment. The as-prepared poly(vinyl alcohol)/cellulose nanofiber hybrid hydrogels show distinct wood-like anisotropy, including oriented molecular fiber bundles and extended grain size, which endows materials with extraordinarily comprehensive mechanical properties of ultimate breaking strength exceeding 40 MPa, strain approaching 250%, and toughness exceeding 60 MJ·m–3, and outstanding tear resistance. Impressively, the breaking strength and toughness of the reswollen preoriented hydrogels approach 10 MPa and 25 MJ·m–3, respectively. In vitro and in vivo tests demonstrate that the reswollen hydrogels do not affect the growth and viability of the cells, nor do they cause the inflammation or rejection of the mouse tissue, implying extremely low biotoxicity and perfect histocompatibility, showcasing bright prospects for application in artificial ligaments or tendons. The strategy provided in this study can be generalized to a variety of biocompatible polymers for the fabrication of high-performance hydrogels with anisotropic structures.