Ionically conductive elastomers are necessary for realizing human−machine interfaces, bioelectronic applications, or durable wearable sensors. Current design strategies, however, often suffer from solvent leakage and evaporation, or from poor mechanical properties. Here, we report a strategy to fabricate ionic elastomers (IHPs) demonstrating high conductivity (0.04 S m −1 ), excellent electrochemical stability (>60,000 cycles), ultrastretchability (up to 1400%), high toughness (7.16 MJ m −3 ), and fast self-healing properties, enabling the restoration of ionic conductivity within seconds, as well as no solvent leakage. The ionic elastomer is composed of in situ formed physically crosslinked poly(2-hydroxyethyl methacrylate) networks and poly-(ethylene glycol) (PEG). The long molecular chains of PEG serve as a solvent for dissolving electrolytes, improve its long-term stability, reduce solvent leakage, and ensure the outstanding mechanical properties of the IHP. Surprisingly, the incorporation of ions into PEG simultaneously enhances the strength and toughness of the elastomer. The strengthening and toughening mechanisms were further revealed by molecular simulation. We demonstrate an application of the IHPs as (a) flexible sensors for strain or temperature sensing, (b) skin electrodes for recording electrocardiograms, and (c) a tough and sensing material for pneumatic artificial muscles. The proposed strategy is simple and easily scalable and can further inspire the design of novel ionic elastomers for ionotronics applications.

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