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The rapid development of wearable electronics has placed higher demands on the design strategies of triboelectric materials. Aerogels have the potential to become advanced triboelectric materials, however, traditional design strategies often require complex processes and additional chemical cross‐linking agents to improve the stability of the gel structure, which limits its practical application. In this work, a scalable and sustainable self‐assembly drive strategy is proposed for the design of bio‐based triboelectric aerogels with multi‐scale winding structures. Interestingly, the autoacceleration effect, which is regarded as “unfavorable” during the autocatalytic polymerization of supramolecules, is rationally exploited to provide the supramolecules within the matrix with an abundance of multiple hydrogen bonds at the same time as their rapid gelation occurs. Thanks to this, the aerogel film exhibits ultra‐high tensile strength (104 MPa) and remains undeformed after resisting an impact of 8000 times its own weight. Highly robust triboelectric aerogel films are used to build wearable self‐powered sensors with ultra‐fast response in complex environments (48 ms), while enabling real‐time interaction between the wearer and the information network. The design idea of “ turning a detriment into an asset ” in this work provides a new idea for the material construction of highly robust wearable sensors. [ABSTRACT FROM AUTHOR]