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

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.