Abstract With rapid advancement in the field of smart technology, reshapeable devices have garnered widespread interest. Liquid‐free flexible materials eliminate the risk of leakage thus enhancing user safety along with being recyclable. However, the poor network fluidity and difficulty in fully disconnecting cross‐links have limited its potential as a reshapeable device. In this work, silver nanoparticles (AgNPs) are doped into a physically cross‐linked dynamic linear polydimethylsiloxane network (PIAU) to develop a closed‐loop recyclable high‐dielectric nanocomposite. This nanocomposite exhibits moderate elastoviscosity‐transition temperature and spatial remodelability based on multiple types of reversible hydrogen bonds and S─Ag bonds. AgNPs are sprayed on the nanocomposite surface to form a conductive coating stabilized by S─Ag bonds at the polymer‐nano interface. Based on this refined assembly, an antibacterial and recyclable triboelectric nanogenerator (TENG) is developed and applied as a high‐precision smart insole. The insole with 16 TENG sensors, resulting in a simplified system that employs machine learning (ML) for personalized motion monitoring, including motion recognition and gait classification. Five algorithm models ensure the high accuracy of the system and enable it to further expand the abnormal gait alarm system. This work presents a new reliable and environmentally friendly strategy for the design of high‐performance sustainable smart devices.