AbstractStretchable organic light-emitting devices are becoming increasingly important in the fast-growing fields of wearable displays, biomedical devices and health-monitoring technology. Although highly stretchable devices have been demonstrated, their luminous efficiency and mechanical stability remain impractical for the purposes of real-life applications. This is due to significant challenges arising from the high strain-induced limitations on the structure design of the device, the materials used and the difficulty of controlling the stretch-release process. Here we have developed a laser-programmable buckling process to overcome these obstacles and realize a highly stretchable organic light-emitting diode with unprecedented efficiency and mechanical robustness. The strained device luminous efficiency −70 cd A⁻¹ under 70% strain - is the largest to date and the device can accommodate 100% strain while exhibiting only small fluctuations in performance over 15,000 stretch-release cycles. This work paves the way towards fully stretchable organic light-emitting diodes that can be used in wearable electronic devices.