Thermally Conductive and Stretchable Elastomers Engineered via Ordered Hydrogen Bonding Interactions

Abstract Elastomers are widely used for their large‐strain reversible stretchability, but their low thermal conductivity limits their applications in thermal management. Increasing the thermal conductivity of elastomers usually involves adding fillers, which deteriorate their stretchability and other desirable properties. Here, a supramolecular structure design strategy is proposed to enhance the thermal conductivity of amorphous elastomers without compromising their stretchability and self‐healing abilities. Supramolecular poly(thioctic acid‐N,N′‐methylenebis acrylamide) elastomers are designed with ordered hydrogen bonding interactions that improve the heat transfer efficiency and maintain excellent stretchability. The resulting elastomers exhibit a thermal conductivity of 0.72 W m⁻¹ K⁻¹, a remarkable stretchability of 427%, a low elastic modulus of 475 kPa, and self‐healing and reprocessing capabilities. This strategy offers a promising alternative for developing thermally conductive elastomers that do not rely on traditional fillers.