Tailoring Structural Uniformity of Cellulosic Triboelectric Aerogel Enabled by Pre‐Nucleation‐Controlled Synthesis

Abstract Cellulose aerogels show promise for self‐powered sensing in high‐temperature environments due to exceptional thermal insulation and intrinsic tribopositivity. However, lacking uniform, efficient inductive transport pathways of charges causes irregular interfacial charge dissipation, thereby inducing unpredictable signal attenuation that significantly degrades the reliability and measurement accuracy of sensors. Herein, a pre‐nucleation‐controlled strategy is proposed to fabricate triboelectric aerogels with tunable pore structures and linear response at high temperatures. By precisely regulating the density of ice nucleation sites, synchronous growth of ice templates at multiple sites guides the self‐assembly of composite nanofibers, forming a uniform and interconnected porous structure. The tailored architecture enhances induced charge density by increasing contact area, optimizes electric field distribution for efficient external charge migration, and suppresses irregular high‐temperature charge dissipation. The optimized PNA exhibits remarkable improvements, with the proportion of dominant pore diameters increasing from 27% to 46% and thermal conductivity reduced to 0.04179 W/m K. The aerogel‐based sensor exhibits a high output power of 3.91 W m − 2 and excellent linear response characteristics (R 2 = 0.993). This work pioneers pore‐structure‐mediated charge transport regulation for triboelectric materials, enabling predictable linear signal decay in extreme environments and providing a universal approach to developing linear‐response wearable sensors.