Thermomechanically Robust Cellulosic Triboelectric Materials Enabled by Interfacial Nano‐Bridge

Abstract Developing high‐performance, wearable electronics that operate reliably in extreme environments is crucial for ensuring life safety, as well as for aerospace and industrial applications. However, existing sensing materials face a trade‐off between mechanical performance and high‐temperature robustness, limiting their performance gains and stability under heat. This study introduces a thermomechanically robust cellulosic triboelectric material with interfacial nano‐bridging that forms a heat‐conducting network. Heat‐conducting nanosheets and nanotubes intertwine with cellulose through noncovalent interactions. A very small amount of carbon nanotubes (2 wt.%) acts as bridging segments that connect the heat‐conducting nanosheets, forming a strong hydrogen‐bond network with cellulose to resist energy dissipation during tensile loading. This yields both high mechanical strength (169 MPa) and high thermal conductivity (12.9 W m −1 K −1 ). The performance far exceeds that of most reported polymer composite sensing materials. As a result, self‐powered devices based on triboelectric materials maintained stable operation at 230 °C, and achieved a high output power of 2.72 W m − 2 . When integrated into wearable self‐powered sensing systems with machine learning, the system achieved a 97% accuracy in motion pose recognition. This work presents a strategy to balance the thermomechanical stability trade‐off and provides a general design pathway for sensing materials suitable for complex operating conditions.