Hydrogen Bonds‐Pinned Entanglement Blunting the Interfacial Crack of Hydrogel–Elastomer Hybrids

Abstract Anchoring a layer of amorphous hydrogel on an antagonistic elastomer holds potential applications in surface aqueous lubrication. However, the interfacial crack propagation usually occurs under continuous loads for amorphous hydrogel, leading to the failure of hydrogel interface. This work presents a universal strategy to passivate the interfacial cracks by designing a hydrogen bonds‐pinned entanglement (Hb–En) structure of amorphous hydrogel on engineering elastomers. The unique Hb–En structure is created by pinning well‐tailored entanglements via covalent‐like hydrogen bonds, which can amplify the delocalization of interfacial stress concentration and elevate the necessary fracture energy barrier within hydrogel interface. Therefore, the interfacial crack propagation can be suppressed under single and cyclic loads, resulting in a high interfacial toughness over 1650 J m⁻² and an excellent interfacial fatigue threshold of 423 J m⁻². Such a strategy universally works on blunting the interfacial crack between hydrogel coating and various elastomer materials with arbitrary shapes. The superb fatigue‐crack insensitivity at the interface allows for durable aqueous lubrication of hydrogel coating with low friction.