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Developing physical hydrogels with advanced mechanical performance and multi-functionalities as alterative materials for load-bearing soft tissues remains a great challenge. Biological protein-based materials generally exhibit superior strength and toughness owing to their hierarchical structures via hydrogen-bonding assembly. Inspired by natural biological protein materials, tannic acid (TA) is exploited as a molecular coupling bridge between cellulose nanocrystals (CNCs) and poly(vinyl alcohol) (PVA) chains for the fabrication of a bio-based advanced physical hydrogel via strong multiple H-bonds. When exposed to mechanical stress, the sacrificial H-bonds can dissipate energy effectively on the molecular scale via dynamic rupture and reformation, endowing these biomimetic hydrogels with remarkable toughness, ultrahigh strength, large elongation, and good self-recoverability, which are much superior to …