<p>Human substance needsśś have been enriched by the development of smart-responsive materials possessing unique responsiveness and mechanical variability. However, acquiring these features in photoresponsive energy-driven elastomers is challengeable but highly desirable. Here, we report fabrication of physically-crosslinked elastomers based on an aliphatic polycarbonate terminated with one azobenzene derivative as the end group. Upon irradiation of UV light, the aliphatic polycarbonate shows unusual mechanical transformation from trans-azobenzene-rich elasticity to cis-azobenzene-rich plasticity, which is contrary to the photo-triggered mechanics of other azopolymers. This indicates that stronger interaction may be established between the terminated cis-azobenzenes and the benzene rings in the side chain of polymer, leading to a higher crosslinking density appeared in the cis-azobenzene-rich sample. This azobenzene-terminated polymer is an energy-driven elastomer, which has photo-switchable supramolecular interactions, showing photo-tunable mechanical properties (the half-life period of the cis-azobenzene is 16.9 h). More interestingly, the photoinduced mechanical change occurs at room temperature, enabling the aliphatic polycarbonate to behave as non-thermally switchable ultra-strong adhesive for different substrates, which is specifically suitable for smart dressings to promote wound healing. This switchable mechanical feature of elastomers may be a reference for smart elastomers towards advanced applications.</p>