<p>Aerogel materials often aim for high elasticity, which typically compromises strength. This challenge in balancing elasticity and strength constrains their applications in wearable circuits, intelligent robots, and flexible sensors. This study presents a topological isomerization strategy based on molecular chain rearrangement to enhance both the elasticity and strength of cellulosic triboelectric aerogels. During the molecular chain rearrangement, ethylenediamine forms competitive hydrogen bonds with hydroxyl groups, disrupting the inherent hydrogen bond network of cellulose and exposing additional active hydroxyl groups. Furthermore, through in situ interfacial polymerization and covalent crosslinking, a polymer topological network is established. This results in a flexible cellulosic triboelectric aerogel with improved elasticity and strength; even after 20,000 cycles of compression, the aerogel exhibited a recoverability exceeding 95% and could support loads over 2000 times its own weight. Concurrently, the transformation of the crystal structure due to the reconstruction of the hydrogen bond network leads to the rearrangement of surface functional groups, which modifies the surface potential and ensures stable triboelectric output across a broad range of temperatures and humidity levels. This strategy provides innovative methods for the design and fabrication of lightweight, ultra-elastic, and extreme-environment-resistant 3D porous materials, which are essential for advancing next-generation sensor devices.</p>