As a nanoscale renewable resource derived from lignocellulosic materials, cellulose nanocrystals (CNCs) have the features of high purity, high crystallinity, high aspect ratio, high Young's modulus, and large specific surface area. The most interesting trait is that they can form the entire films with bright structural colors through the evaporation‐induced self‐assembly (EISA) process under certain conditions. Structural color originates from micro‐nano structure of CNCs matrixes via the interaction of nanoparticles with light, rather than the absorption and reflection of light from the pigment. CNCs are the new generation of photonic liquid crystal materials of choice due to their simple and convenient preparation processes, environmentally friendly fabrication approaches, and intrinsic chiral nematic structure. Therefore, understanding the forming mechanism of CNCs in nanoarchitectonics is crucial to multiple fields of physics, chemistry, materials science, and engineering application. Herein, a timely summary of the chiral photonic liquid crystal films derived from CNCs is systematically presented. The relationship of CNC, structural color, chiral nematic structure, film performance, and applications of chiral photonic liquid crystal films is discussed. The review article also summarizes the most recent achievements in the field of CNCs‐based photonic functional materials along with the faced challenges.