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.