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Recently, circularly polarized organic light‐emitting diodes (CP‐OLEDs) fabricated with thermally activated delayed fluorescence (TADF) emitters are developed rapidly. However, most devices are fabricated by vacuum deposition technology, and developing efficient solution‐processed CP‐OLEDs, especially nondoped devices, is still a challenge. Herein, a pair of triptycene‐based enantiomers, (S,S)‐/(R,R)‐TpAc‐TRZ, are synthesized. The novel chiral triptycene scaffold of enantiomers avoids their intermolecular π–π stacking, which is conducive to their aggregation‐induced emission characteristics and high photoluminescence quantum yield of 85% in the solid state. Moreover, the triptycene‐based enantiomers exhibit efficient TADF activities with a small singlet‐triplet energy gap (ΔEST) of 0.03 eV and delayed fluorescence lifetime of 1.1 µs, as well as intense circularly polarized luminescence with dissymmetry factors (|gPL|) of about 1.9 × 10−3. The solution‐processed nondoped CP‐OLEDs based on (S,S)‐/(R,R)‐TpAc‐TRZ not only display obvious circularly polarized electroluminescence signals with gEL values of +1.5 × 10−3 and −2.0 × 10−3, respectively, but also achieve high efficiencies with external quantum, current, and power efficiency up to 25.5%, 88.6 cd A−1, and 95.9 lm W−1, respectively. [ABSTRACT FROM AUTHOR]

A strategy of chiral donor–acceptor copolymerization is proposed to develop chiral nonconjugated polymers with thermally activated delayed fluorescence (TADF). Based on this strategy, two pairs of chiral polymers (R,R)‐/(S,S)‐pTpAcDPS and (R,R)‐/(S,S)‐pTpAcBP were synthesized. The alternating copolymerization of the chiral donors and acceptors could effectively separate the frontier molecular orbitals, which made the polymers show small ΔEST of 0.01–0.03 eV and efficient TADF properties. Moreover, the polymers also showed the quantum yield of up to 92 % and the circularly polarized luminescence. The solution‐processed circularly polarized organic light‐emitting diodes showed circularly polarized electroluminescence signals with high external quantum efficiencies of up to 22.1 % and maximum luminance of up to 34350 cd m−2. This is the first report of CP‐OLEDs based on chiral TADF polymer, which provides a useful and valuable guidance for the development of high‐efficiency CPEL polymers. [ABSTRACT FROM AUTHOR]