Bioinspired Robust Aramid Triboelectric Aerogels with Vertically Oriented Architecture Enabled by Magnetization Effects

Abstract Many natural organisms utilize vertically oriented bristles to gain environmental information, and replicating these precisely oriented structures in sensing materials is crucial for improving sensing performance. Building ordered oriented architectures while maintaining the material's mechanical robustness remains challenging. Inspired by the vertically bristle structure of gecko toes, this study proposes a magnetic‐thermal synergistic strategy for fabricating robust aramid nanofiber aerogels with a vertically oriented spatial structure. Under the influence of magnetic torque and magnetic attraction, magnetic carbon nanotubes spontaneously align to form an ordered vertically oriented architecture (direction fit of 96%). This architecture enhances the sensing signal intensity of the aerogel by 64% by inducing surface charge migration. The thermally crosslinked effect enhances the bonding strength between aerogel fiber networks, enabling the aerogel to achieve a compressive strength of 682 kPa (80% compressive strain). This surpasses the compressive strength of aramid fiber aerogels reported to date. The vertically oriented aerogel is assembled into a self‐powered pressure sensor, achieving a signal recognition rate of 98.2% with machine learning assistance. This study proposes a non‐invasive spatial microstructure regulation strategy, offering new insights into the construction of anisotropic structural materials.