Super-Strong, Nonswellable, and Biocompatible Hydrogels Inspired by Human Tendons

Fabricating artificial materials that mimic the structures and properties of tendons is of great significance. Possessing a tensile stress of approximately 10.0 MPa and a water content of around 60%, human tendons exhibit excellent mechanical properties to support daily functions. In contrast to tendons, most synthetic hydrogels with similar water content typically exclude qualified strength, swelling resistance, and biocompatibility. Herein, a facile strategy based on poly(vinyl alcohol) (PVA) and tannic acid (TA) is demonstrated to tackle this problem via a combination of sequential steps including freezing–thawing PVA aqueous solutions to form crystalline regions, prestretching and air drying in confined conditions to induce anisotropic structures, soaking in TA solutions to form multiple hydrogen bondings between PVA and TA, and finally dialyzing against water for the removal of residual TA molecules and the rearrangements and homogenization of multiple hydrogen bonds. The obtained PVA hydrogels possess hierarchically anisotropic structures, where the alignment of PVA bundles promotes high modulus, while the hydrogen bonding between PVA and TA endows them with an energy dissipation mechanism. Benefitting from the synergy of material composition and structural engineering, the obtained hydrogel displays super-strong mechanics (a tensile stress of 19.3 MPa and a toughness of 32.1 MJ/m³), outperforming most tough hydrogels. Remarkably, this hydrogel demonstrates excellent swelling resistance. It barely expands after immersion in deionized water, phosphate-buffered saline (PBS), and SBF aqueous solutions for 7 days with the strength and volume nearly the same as their initial values. All of the features, combined with excellent cytocompatibility, make it an ideal material for biotechnological and biomedical applications.