Purely organic TADF emitters have rapidly developed in recent years and TADF has become one of the most promising achievement for highly efficient OLEDs. Apart from the advantages such as...

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.