Stretchable, Ultratough, and Intrinsically Self‐Extinguishing Elastomers with Desirable Recyclability

Advanced elastomers are increasingly used in emerging areas, for example, flexible electronics and devices, and these real-world applications often require elastomers to be stretchable, tough and fire safe. However, to date there are few successes in achieving such a performance portfolio due to their different governing mechanisms. Herein, a stretchable, supertough, and self-extinguishing polyurethane elastomers by introducing dynamic π-π stacking motifs and phosphorus-containing moieties are reported. The resultant elastomer shows a large break strain of ≈2260% and a record-high toughness (ca. 460 MJ m⁻³ ), which arises from its dynamic microphase-separated microstructure resulting in increased entropic elasticity, and strain-hardening at large strains. The elastomer also exhibits a self-extinguishing ability thanks to the presence of both phosphorus-containing units and π-π stacking interactions. Its promising applications as a reliable yet recyclable substrate for strain sensors are demonstrated. The work will help to expedite next-generation sustainable advanced elastomers for flexible electronics and devices applications.