Ion-conductive　elastomers　have　emerged　as　ideal　candidates　for　ionic　skin　and　wearable　devices　due　to　their　intrinsic　stretchability　and　excellent　electrical　properties.　Despite　continuous　efforts　in　this　field,　strain-stiffening,　robust　yet　compliant　ionic　elastomers　are　still　unattainable　due　to　the　limited　intermolecular　interactions,　restricting　their　reliability　and　durability　in　practical　applications.　Inspired　by　the　interwoven　collagen　fiber　network　and　synergistic　non-covalent　interaction　in　the　dermis,　an　immense　strain-stiffening,　ultra-stretchable,　highly　tough,　and　elastic　ionic　elastomer　are　reported　by　introducing　the　metal–oxygen　interactions　into　the　highly　entangled　network.　The　ionic　elastomers　also　show　intriguing　self-healing　ability,　high　adhesion,　and　environmental　tolerance,　contributed　by　the　dynamic　synergistic　noncovalent　interactions.　The　prepared　ionic　skin　displays　sensitive　and　stable　responses　to　temperature　and　strain.　This　work　demonstrates　a　new　design　strategy　for　fabricating　high-performance　ionic　elastomers　with　excellent　mechanical　and　electrical　properties,　showing　great　prospects　in　wearable　and　flexible　devices.　©　2024　Wiley-VCH　GmbH.