Mechanically Robust and Self‐Healing Sustainable Solid‐State Ion‐Conductive Elastomer for Near‐Infrared‐Driven Noncontact Sensing

ABSTRACT Stretchable solid‐state ionic conductive elastomers (SICEs), serving as essential materials for ionotronic devices, exhibit great promise in emerging applications in electronic skin, soft robotics, especially in wearable sensors. Nevertheless, the development of such materials with high strength, self‐healing, and ionic conductivity remains highly desirable yet challenging, as simultaneously integrating these properties is often hindered by intrinsic trade‐offs among molecular chain dynamics and desired functions. Herein, we develop a SICE featuring a natural rubber‐based segregated network, in which latex particles are encapsulated by carboxylated cellulose nanofibers, polydopamine, and lithium bis(trifluoromethanesulfonyl)imide. The formation of integrated dense interfacial hydrogen and lithium bonds among the components leads to a robust interface and superior integral architecture, delivering an unprecedented combination of properties: a tensile strength of 6.23 MPa, a room‐temperature self‐healing efficiency of 98%, and an ionic conductivity of 4.15 × 10 − 3 S·m −1 . Such performance substantially outperforms the most state‐of‐the‐art bio‐based counterparts, noting that all main components are derived from bio‐based resources. Furthermore, the polydopamine imparts photothermal conversion capability, enabling not only remote‐triggered rapid self‐healing but also non‐contact sensing via near‐infrared light‐mediated thermal stimulation. This study advances a sustainable and remotely controllable platform based on bio‐based SICEs, opening new avenues for next‐generation intelligent flexible electronics.