Cellulose nanocrystal(CNC)can self-assemble and arrange at specific concentrations,imparting unique optical properties to the system.This paper investigated the effects of sealed deposition time and CNC concentration on the form-ation and alignment of cholesteric liquid crystals within the naturally dried films by analyzing the changes of CNC films in macroscopic color,UV-vis spectra,polarization optics,microscopic morphology,and crystal structure to elucidate the mechanism of CNC self-assembly behavior during the formation of CNC films.The results showed that when the sealed deposition time was extended to 48 h,the structural color development range and the long-range ordering of the cholesteric phase structure of CNC films were considerably enhanced.As the concentration increased,the CNC particle spacing decre-ased,the torsion angle between neighboring particles increased,and the pitch was compressed,decreasing from 480 nm to 344 nm.The results of polarized light microscopy analysis demonstrated that the sealed deposition treatment had a signi-ficant advantage in the formation of long-range ordered cholesteric phase structure in high-concentration CNC suspensions.The results of this research indicated that prolonging the sealed deposition time and increasing the CNC concentration could enhance the improvement of long-range orderliness in the films and promote the formation of cholesteric phase structural domains.This further improved the scientific basis for the preparation of CNC-based smart packaging materials and had a positive effect on the development of new visual food packaging and inspection materials.