Cable-Confined Elastomers with Spatially Decoupled Sheath-Core Architecture for Highly Efficient Intrinsically Stretchable Organic Light-Emitting Diodes

The longstanding compromise between high electroluminescence efficiency and extreme mechanical stretchability has fundamentally constrained optoelectronic advancement for decades. Herein, we introduce an innovative cable-confined design strategy that spatially decouples charge carrier transport (functional sheath) from strain dissipation (dissipative core) in intrinsically stretchable electroluminescent elastomers. Rigid thermally activated delayed fluorescence (TADF) sheaths are covalently integrated around polybutadiene cores via one-pot random copolymerization. The resulting free-standing elastomers retain high electroluminescence efficiency while demonstrating exceptional stretchability. Corresponding organic light-emitting diodes (OLEDs) achieve a current efficiency of 26.3 cd A–1 and an external quantum efficiency of 11.9%, the highest values reported for stretchable electroluminescent materials to date. This work establishes a transformative paradigm for high-performance intrinsically stretchable displays and electronics.