The work aims to develop and evaluate a micro-nano composite film packaging material based on polylactic acid (PLA) and nanofibrillated cellulose (NFC) to enhance the preservation effect of fruits and vegetables and reduce the environmental impact. Polyethylene terephthalate (PET) films were used to replace fruits and vegetables for quantitative testing. The effects of the spraying times of a mixture of 0.5% NFC and PLA micro-particles of different concentrations and particle sizes on the oxygen permeability, water vapor permeability and radiation heat dissipation effect of PET films were studied. The results showed at 5 times of spraying of 0.5% NFC, the oxygen and water vapor permeability of the composite film were the lowest. Adding PLA micro-particles of moderate concentration and particle size (such as 30 μm) to cellulose could enhance the oxygen barrier performance and reduce the water vapor permeability of PET films. Five times of spraying were the balance point, and excessive spraying would instead reduce the moisture resistance. The addition of NFC and PLA micro-particles gave PET films a certain radiation heat dissipation effect. In conclusion, NFC and PLA micro-particles of appropriate concentrations, particle sizes and spray times can significantly improve the performance of the composite film. This micro-nano composite film enhances the oxygen and moisture barrier performance by improving the uniformity of the cellulose film and has a potential radiation cooling effect, providing a strategy for the development of micro-packaging materials for fruit and vegetable preservation.