Abstract Purely organic molecules with room‐temperature phosphorescence (RTP) are potential luminescent materials with high exciton utilization for organic light‐emitting diodes (OLEDs), but those exhibiting superb electroluminescence (EL) performances are rarely explored, mainly due to their long phosphorescence lifetimes. Herein, a robust purely organic RTP molecule, 3,6‐bis(5‐phenylindolo[3,2‐a]carbazol‐12(5H)‐yl)‐xanthen‐9‐one (3,2‐PIC‐XT), is developed. The neat film of 3,2‐PIC‐XT shows strong green RTP with a very short lifetime (2.9 μs) and a high photoluminescence quantum yield (72 %), and behaviors balanced bipolar charge transport. The RTP nature of 3,2‐PIC‐XT is validated by steady‐state and transient absorption and emission spectroscopies, and the working mechanism is deciphered by theoretical simulation. Non‐doped multilayer OLEDs using thin neat films of 3,2‐PIC‐XT furnish an outstanding external quantum efficiency (EQE) of 24.91 % with an extremely low roll‐off (1.6 %) at 1000 cd m −2 . High‐performance non‐doped top‐emitting and tandem OLEDs are also achieved, providing remarkable EQEs of 24.53 % and 42.50 %, respectively. Delightfully, non‐doped simplified OLEDs employing thick neat films of 3,2‐PIC‐XT are also realized, furnishing an excellent EQE of 17.79 % and greatly enhanced operational lifetime. The temperature‐dependent and transient EL spectroscopies demonstrate the electrophosphorescence attribute of 3,2‐PIC‐XT. These non‐doped OLEDs are the best devices based on purely organic RTP materials reported so far.
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