Abstract
Silicone elastomers are essential for wearable electronics and soft robotics, but conventional PDMS is based on non-recyclable monomer platforms, limiting sustainability. Here, we report a chemically recyclable silicone elastomer with high elasticity enabled by introducing new silicone monomers and network topology. Recyclable vinyl- and hydride-terminated silicone macromonomers form a topologically interlocked ring network via hydrosilylation without permanent covalent crosslinks, resulting in elastic behavior governed by chain entanglements and topological constraints. The system allows selective depolymerization into cyclic monomers and subsequent repolymerization, enabling closed-loop chemical recycling. As a result, the elastomer exhibits elongation exceeding 2000%, low hysteresis, and a monomer recovery yield of 76%. This work demonstrates that controlling silicone monomer design and ring-based topology enables sustainable, high-performance silicone elastomers.