Zwitterionic Ionogels Resolving the Trade-Off Between Mechanical Strength and Autonomous Self-Healing for Iontronics

Abstract Simultaneously achieving mechanical robustness and autonomous self-healing in ionogels remains a fundamental challenge for durable, skin-like electronics. Conventional approaches often improve mechanical strength by introducing rigid or densely cross-linked polymer networks, but such strategies inevitably restrict polymer chain mobility and hinder dynamic bond reconfiguration required for healing. Here, a zwitterionic side-chain engineered tough ionogel (ZESTI) is developed to overcome this trade-off through molecular-level design. Hydrophilic zwitterions are covalently grafted onto a hydrophobic polyurethane backbone to preferentially interact with the ionic liquid through ion–dipole interactions and thereby regulate its distribution. This architecture simultaneously facilitates dipole–dipole interactions for mechanical reinforcement and ion–dipole coordination for efficient self-healing under ambient conditions. As a result, ZESTI exhibits an exceptional combination of tensile strength (10.40 MPa), stretchability (1606%), toughness (56.03 MJ m −3 ), and ambient self-healing efficiency exceeding 83%, while maintaining high ionic conductivity via enhanced ion hopping. When constructed as a self-reporting packaging interface, ZESTI provides stable protection and state perception under sharp contact and restores signal output after mechanical damage through self-healing. This work offers a generalizable design strategy that reconciles mechanical toughness with dynamic functionality in ionogels, establishing a general design paradigm for next-generation self-sustaining iontronic devices.