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Conventional colored radiative cooling (ColPRC) has a single color and limited reflection of visible light bands, which affects its radiative cooling effect, and the introduction of multiple photonic crystal structures can improve its radiative cooling performance. Therefore, in this study, a composite film was established by cross‐linking cellulose nanocrystals (CNC) with CO2‐based waterborne polyurethane (WPU) to obtain multistage structural colors. X‐ray diffraction pattern, thermogravimetric analysis, scanning electron microscopy, spectral analysis, and so on were used to examine the structure and properties of the films. The results showed that with the increase of CNC content, the color shifted blue, the crystallinity increased, the flame retardancy increased, but the thermal stability decreased; the addition of WPU assists in resisting moisture; the reflectivity of the multistage structured films is improved in the VIS–NIR range compared with the monochromatic films (an average increase of 5%), which helps to reduce solar irradiation in the visible wavelengths; high emissivity (≈90%) in the atmospheric window, which facilitates deep‐space heat exchange. The maximum temperature difference of the multistage structural color film can reach 6°C under strong solar irradiation. This research can be applied in photovoltaic devices or outdoor thermal management to provide new ways to address human energy efficiency. [ABSTRACT FROM AUTHOR]