In this work, we studied the formation and properties of composite films coassembled by cellulose nanocrystals (CNCs) and bovine serum albumin-stabilized gold nanoclusters (BSA-AuNCs). The influences of the BSA-AuNC concentration on the structure and optical properties of CNC-based composite films were further studied. It was found that the composite film retained the chiral nematic structure and optical activity. The self-assembled CNC and BSA-AuNC helical superstructures can produce strong, left-handed, circularly polarized luminescence with dissymmetry factors up to 0.287. Meanwhile, the third component, polyethylene glycol, was introduced without affecting the structural color and fluorescence characteristics of the composite film to enhance the flexibility of the film. The simplicity of the film preparation, the abundance of CNCs, and the flexibility and stability of the composite films pave the way for the production of functional materials with integrated functions.