Multiscale Structural Strong yet Tough Triboelectric Materials Enabled by In Situ Microphase Separation

Abstract Lightweight green polymer materials with exceptional toughness, high strength, and excellent ductility represent ideal candidates for enabling next‐generation sustainable flexible electronics. However, the conflicting properties of material strength and toughness present a significant challenge in achieving an optimal combination of both attributes. In this study, a strong yet tough polymeric triboelectric material is prepared by constructing a multiscale reinforced network based on a nonsolvent‐induced microphase separation strategy. The synergistic enhancement of strength and toughness is achieved by reinforcing non‐covalent interactions within the polymer and constructing nanofibrous networks. The resulting triboelectric materials exhibited remarkable fracture toughness (78.6 MJ m⁻³), high tensile strength (42.5 MPa), an improvement in triboelectric output (71%), and promising recyclability. The integrated triboelectric wearable sensor maintained robust output signals. This study provides a novel solution for coordinating the conflicts between strength and toughness in heterogeneous polymer materials, showing significant potential in expanding their applications in flexible electronics and self‐powered sensing technologies.