Integrating proteins into a hydrogel network enables its good bioactivity as an ECM environment in biorelative applications. Although extensive studies on preparing protein hydrogels have been carried out, the reported systems commonly present very low mechanical strength and weak water-rentention capacity. Learning from the astringent mouthfeel, we report here a protein engineered multinetwork physical hydrogel as TA-PVA/BSA. In a typical case, the BSA protein-integrated poly(vinyl alcohol) (PVA) solution is treated by the freeze-thaw method and forms the first hydrogel network, and tannic acid (TA) then cross-links with BSA proteins and PVA chains to form the secondary hydrogel network based on the noncovalent interaction (hydrogen bond and hydrophobic interaction). The as-prepared TA-PVA/BSA composite hydrogel is a pure physically cross-linking network and possesses ultrahigh tensile strength up to ∼9.5 MPa but is adjustable, relying on the concentration of TA and BSA. Moreover, its mechanical strength is further improved by prestretching induced anisotropy of mechanical performance. Because of its controllable and layered structure as skin, the composite hydrogel presents good water-retention capacity compared to traditional high strength hydrogels. This work demonstrates a novel method to design high mechanical strength but layered physical cross-linking hydrogels and enables us to realize their biorelative applications.