Tough, Swelling-Resistant, Self-Healing, and Adhesive Dual-Cross-Linked Hydrogels Based on Polymer–Tannic Acid Multiple Hydrogen Bonds

We demonstrate a facile and universal strategy in the fabrication of dual-cross-linked (DC) single network hydrogels with high toughness, “nonswellability”, rapid self-healing, and versatile adhesiveness based on polymer–tannic acid (TA) multiple hydrogen bonds. Two widely used hydrogels, physically cross-linked poly­(vinyl alcohol) and chemically cross-linked polyacrylamide, have been transformed to TA-based DC hydrogels by dipping the corresponding aerogels into TA solution. The second cross-link via multiple polymer–TA hydrogen bonds effectively suppresses the crack propagation, resulting in both DC gels with high mechanical strength. But these two TA-based DC hydrogels go through different deformation mechanisms during the stretching based on analyzing their stress–strain curves using the Mooney–Rivlin equation. Moreover, these DC hydrogels are swelling-resistant, with strong toughness, good self-recoverability, rapid self-healing, and versatile adhesiveness. This work provides a simple route to fabricate multifunctional DC hydrogels, hopefully promoting their applications as biomedical materials.