In this article, UV-curable liquid CBU226 was firstly employed as the shell material to microencapsulate cholesteric liquid crystals (CLCs) by a combined technique of solvent evaporation and photopolymerization. Microcapsule properties depend on the sequence of photopolymerization and solvent evaporation process during preparation. Solvent-evaporation-induced-phase-separationphotopoly-merization process could produce microcapsules with high core loading and spherical core/shell structure. Specifically, spherical CLC microcapsules with mononuclear structure, smooth surface, and high CLC loading (97.34wt%) were prepared. After drying, the microcapsules could easily deform to nonspherical geometry and exhibit vivid color, showing great potential for the application of display devices.