Chemical Compatibility Enables Dual‐Role Carbonized Polymer Dots for Robust, Highly Stretchable, and Rapidly Self‐Healing Room‐Temperature Phosphorescent Elastomers

ABSTRACT Achieving persistent room‐temperature phosphorescence (RTP), mechanical robustness, high stretchability, and rapid self‐healing in a single elastomer is challenging because triplet confinement and load bearing require restricted interactions, whereas deformation and repair require chain mobility and reversible bonding. Here, low‐carbonization carbonized polymer dots (CPDs) are directly incorporated into a chemically compatible poly( N,N ‐dimethylacrylamide‐co‐methoxy poly(ethylene glycol) acrylate) elastomer (DM 6 ). Chemical compatibility activates the native dual role of CPDs: their partially carbonized domains serve as intrinsic RTP centers, while their polymer‐like surfaces form reversible hydrogen bonds with DM 6 , simultaneously providing local triplet confinement and dynamic physical crosslinking. The resulting DM 6 /CPDs‐ 8 exhibits a tensile strength of 6.14 MPa, a fracture strain of 923%, and 94.1% strength recovery after only 30 s of contact at room temperature without heating or external healing agents. Across the composition series, the phosphorescence lifetime reaches 538.1 ms, and the fracture energy reaches 43.2 kJ m − 2 , while DM 6 /CPDs‐ 8 maintains tan δ > 1 from 0.02 to 300 Hz. This compatibility‐enabled integration provides a direct route to mechanically robust, highly stretchable, rapidly self‐healing RTP elastomers with high crack tolerance and broadband damping.