Design and preparation of gels with excellent mechanical properties has garnered wide interest at present. In this paper, preparation of polyvinyl alcohol (PVA)–tannic acid (TA) gels with exceptional properties is documented. The crystallization zone and hydrogen bonding acted as physical crosslinkages fabricated by a combination of freeze–thaw treatment and a tannic acid compound. The effect of tannic acid on mechanical properties of prepared PVA–TA gels was investigated and analyzed. When the mass fraction of PVA was 20.0 wt% and soaking time was 12 h in tannic acid aqueous solution, tensile strength and the elongation at break of PVA–TA gel reached 5.97 MPa and 1450%, respectively. This PVA–TA gel was far superior to a pure 20.0 wt% PVA hydrogel treated only with the freeze–thaw process, as well as most previously reported PVA–TA gels. The toughness of a PVA–TA gel is about 14 times that of a pure PVA gel. In addition, transparent PVA–TA gels can effectively prevent ultraviolet-light-induced degradation. This study provides a novel strategy and reference for design and preparation of high-performance gels that are promising for practical application.
