Mechanically Resilient Bioinspired Aerogels Enabled by Cross‐Scale Interfacial Engineering for Multifunctional Wearable Electronics

ABSTRACT Rapid advancement of wearable electronics, the Internet of Things, and artificial intelligence has generated a growing demand for flexible sensors capable of reliable and high‐precision pressure monitoring under complex conditions. However, traditional piezoresistive sensors often suffer from sensitivity degradation and structural fatigue caused by moisture exposure and long‐term cyclic loading. Here, we report a ternary composite aerogel‐based piezoresistive sensor composed of tobacco stem‐derived TEMPO‐oxidized cellulose nanofibers (TTOCNFs), MXene, and polymethylsilsesquioxane (PMSQ) through cross‐scale interfacial engineering. In this design, TTOCNFs form a flexible skeleton, MXene establishes an efficient conductive network, and PMSQ reinforces the framework while imparting hydrophobicity, mitigating moisture‐induced performance degradation. An ice‐templating strategy further constructs a honeycomb‐like skeleton, enabling efficient stress distribution under mechanical deformation. Benefiting from these structural and interfacial synergies at different scales, the sensor exhibits high sensitivity (1612.8 kPa −1 ), broad detection range (2.4 Pa–48.8 kPa), rapid response and recovery (117 and 80 ms), and outstanding cycling stability (>1000 cycles), while maintaining reliable performance in humid environments. It enables high‐fidelity monitoring of subtle physiological signals and human motions, demonstrating strong potential for health monitoring and human‐machine interaction. This work provides a scalable and sustainable design strategy for environmentally robust aerogel‐based pressure sensors toward smart wearable electronics.