Structural color coatings with brilliant color is important in practical applications, such as aesthetic decoration, bionic skins, colorimetric sensors, and other color‐related fields. However, the intrinsic conflict between fast self‐assembly and bright structural color hinders their widespread applications. Here, cholesteric liquid crystal elastomer (CLCE) coatings with brilliant color and mechanochromic response are developed by spraying the cholesteric liquid crystal (CLC) paints followed by evaporation‐induced self‐assembly (EISA) and photocuring. The Marangoni flow within the paints, which drives the orientation of liquid crystal molecules along the flow track in the EISA process, is found to be crucial for achieving both rapid self‐assembly time (60 s) and high reflectivity structural color (42%). The as‐prepared CLCE coatings present uniform structural colors, circularly polarized reflection, and mechanochromic response. Several proofofconcept applications are also demonstrated, including patterned CLCE coatings on flat substrates, fully covered CLCE coatings on 3D objects, and non‐spectral colors via additive mixing method. The research disclosed herein provides unprecedented levels of efficiency and reliability for preparing structural color coatings.