dissymmetry factor (g PL) (defined as 2(I L − I R)/(I L + I R) where I is the emission intensity), which takes a value between −2 and +2. [3] In addition, good emission efficiency is clearly important, especially in the condensed state. Over the past decades, several strategies to realize efficient CPL-active materials have been developed [4] and much work has concentrated on determining the most efficient method of introducing a chiral center into the emissive material. [5] To date, various kinds of chiral materials, including polymers and small molecules, [6] have been developed for CPL. However, most of the reported CPLactive emitters are fluorescent materials which therefore have an intrinsic internal quantum efficiency (IQE) of 25%, [7] leading to a limitation in the device. To enhance the IQE of the CPL emitter, various complexes with different transition metals were explored recently as they offer the prospect of quantitative IQE. [8] For these circularly polarized organic light-emitting diodes (CP-OLEDs), device performance, and the luminescence dissymmetry factor (g EL) of circularly polarized electroluminescence (CPEL) were two main aspects to evaluate the level of device. [9] To date, few examples have been reported with both high emission efficiency in solution-processable CP-OLED and a large luminescence dissymmetry factor. For example, Di Bari et al. reported a CP-OLED based on chiral Eu-complexes and its 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.