Abstract Circularly polarized luminescence (CPL) is of interest due to its wide potential application in semiconductors. To balance the emission efficiency and luminescence dissymmetry factor ( g PL ) of a CPL emitter, in this context, two chiral, phosphorescent and liquid‐crystalline cyclometalated platinum complexes, abbreviated R ‐Pt and S ‐Pt, are prepared. The complexes, which show an intense green emission at 504 nm both in solution and in the solid state, contain a simple, ortho ‐metalated 2‐phenylpyridine unit functionalized with a chiral 2‐octanol chain, with liquid crystallinity being induced by modifying the β‐diketonato ligand with mesogenic groups. Interestingly, both the chiral smectic (SmA*) and nematic (N*) phases are found by a combination of polarized optical microscopy, differential scanning calorimetry, and small‐angle X‐ray scattering. By annealing, distinct CPL emission is achieved in the solid state with a g PL around 0.02. Employing the chiral platinum complexes as the dopant, solution‐processable organic light‐emitting diodes present an external quantum efficiency of 11.3% and strong, circularly polarized electroluminescence with an extremely high luminescence dissymmetry value ( g EL ) of 0.06 after annealing at 100 °C. This work opens an avenue for designing CPL‐active emitters with high emission efficiency and high dissymmetry factor.