Abstract: In recent years, circularly polarized luminescent materials have received extensive attention in the field of optoelectronic and spintronic devices due to their unique photophysical properties. However, the existing systems generally face critical problems such as low asymmetry factor and difficult chiral modulation. In this study, multicolor fluorescence-emitting CsPbX₃ chalcogenide nanocrystals were prepared by ultrasonication. Cellulose nanocrystal/glucose (CNC/Glu) composite films were prepared by modulating the glucose doping concentration. Bilayer devices with excellent circularly polarized luminescence performance were constructed by compositing chiral nematic phase optical films of cellulose nanocrystals with lead halide chalcogenide materials. The results of circularly polarized fluorescence spectroscopy tests showed that the photonic bandgap center wavelength of the cellulose chiral film was spectrally matched with the emission peak (522 nm) of the CsPbBr₃ chalcogenide fluorescent material when the glucose doping amount was 30%. The luminescence asymmetry factor of this composite system reaches |1.8|, which is a significant improvement over the conventional material. The chiral modulation of circularly polarized fluorescence can be achieved by different excitation modes. In terms of device structure design, this study innovatively adopts a modular two-layer architecture: the physical separation of the chiral modulation layer and the luminescence layer avoids the influence of chemical modification on the performance of circularly polarized luminescent materials in the traditional method, and significantly improves its feasibility as a circularly polarized luminescent device.