Reprocessable Supramolecular Elastomers of Poly(Siloxane–Urethane) via Self‐Complementary Quadruple Hydrogen Bonding

Abstract Supramolecular silicone materials are promising candidates toward sustainable and recyclable applications. Herein, quadruple hydrogen bond motifs are introduced into the main chain of polysiloxane for the first time, providing a new type of supramolecular silicone elastomers. This structural design enables the well‐defined spacing length between ureidopyrimidinone (UPY) units, exercising better control over polymer network structure. The obtained materials exhibit elastomeric properties and robust reprocessability, and can be further developed into europium (Eu)‐coordinated elastomers with interesting water‐responsive luminescence. It is highly anticipated that this work will broaden the scope and application of silicone‐based sustainable materials.