Blue thermally activated delayed fluorescent emitters are promising for the next generation of organic light-emitting diodes, yet their performance still cannot meet the requirements for commercialization. Here we establish a design rule for highly efficient and stable thermally activated delayed fluorescent emitters by introducing an auxiliary acceptor that could delocalize electron distributions, enhancing molecular stability in both the negative polaron and triplet excited state, while also accelerating triplet-to-singlet up-conversion and singlet radiative processes simultaneously. Proof-of-concept thermally activated delayed fluorescent compounds, based on a multi-carbazole-benzonitrile structure, exhibit near-unity photoluminescent quantum yields, short-lived delays and improved photoluminescent and electroluminescent stabilities. A deep-blue organic light-emitting diode using one of these molecules as a sensitizer for a multi-resonance emitter achieves a remarkable time to 95% of initial luminance of 221 h at an initial luminance of 1,000 cd m-2, a maximum external quantum efficiency of 30.8% and Commission Internationale de l'Eclairage coordinates of (0.14, 0.17).
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