Robust interfacial compliance is essential for long-term physiological monitoring via skin-mountable ionic materials. Unfortunately, existing epidermal ionic skins are not compliant and durable enough to accommodate the time-varying deformations of convoluted skin surface, due to an imbalance in viscosity and elasticity. Here we introduce a self-compliant ionic skin that consistently works at the critical gel point state with almost equal viscosity and elasticity over a super-wide frequency range. The material is designed by leveraging hierarchical hydrogen bond association, allowing for the continuous release of polymer strands to create topological entanglements as complementary crosslinks. By embodying properties of rapid stress relaxation, softness, ionic conductivity, self-healability, flaw-insensitivity, self-adhesion, and water-resistance, this ionic skin fosters excellent interfacial compliance with cyclically deforming substrates, and facilitates the acquisition of high-fidelity electrophysiological signals with alleviated motion artifacts. The presented strategy is generalizable and could expand the applicability of epidermal ionic skins to more complex service conditions.

强大的界面顺应性对于通过可贴肤离子材料进行长期生理监测至关重要。不幸的是，由于粘度和弹性的不平衡，现有的表皮离子皮肤不够柔和耐用，无法适应波纹皮肤表面的时变变形。在这里，我们介绍了一种自顺应性离子皮肤，它在临界凝胶点状态下始终工作，在超宽频率范围内具有几乎相等的粘度和弹性。该材料是通过利用分层氢键缔合而设计的，允许聚合物链的连续释放，从而产生拓扑缠结作为互补交联。通过体现快速应力松弛、柔软性、离子导电性、自愈性、不敏感缺陷、自粘附和防水等特性，这种离子皮肤促进了与周期性变形基材的出色界面柔应性，并有助于获得高保真电生理信号并减轻运动伪影。所提出的策略是可推广的，并且可以将表皮离子皮肤的适用性扩展到更复杂的使用条件。