Unstable hydrogel-substrate interfaces and defunctionalization at low temperature severely restrict versatile applications of hydrogel-based systems. Herein, various chitosan-polyacrylamide double-network (CS-PAM DN) ionic hydrogels were chemically linked with diverse substrates to construct robust and anti-freezing hydrogel-substrate combination, wherein the destructible CS physical network rendered effective energy dissipation mechanism to significantly enhanced the cohesion of hydrogels and the covalent linkage between PAM network with substrate surface strongly improved the interfacial adhesion. The synergistic effects enabled the CS-PAM DN hydrogels to be tightly bonded on diverse metals and inorganics. Impressively, the hydrogel-substrate combinations were freezing tolerant to well-maintain high interfacial toughness at low temperature. Notably, due to the high toughness and conductivity of hydrogel-metal interface, the hydrogel-metal combination can be utilized as a multi-model flexible sensor to detect strain and pressure within broad temperature range. This work may provide a platform for construction and emerging application of robust, anti-freezing and stable-performance hydrogel-based systems.
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