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[Display omitted] • The modified atmosphere packaging is constructed by using nanoMOFs as gas switches. • The gas switches can control the selective CO 2 /O 2 permeation at the molecular level. • The 1.6 % HKUST-1/CMC/Zein has the best the CO 2 /O 2 selectivity of 8.65 ± 1.63. • The 1.6 % HKUST-1/CMC/Zein can keep the freshness of mango for at least 7 days. The storage atmosphere of low O 2 and high CO 2 concentration can regulate plant cell respiration and microbial growth, which plays a crucial role in food preservation. However, traditional modified atmosphere packaging (MAP) cannot accurately control gas penetration. In this study, a novel strategy for accurately controlling the selective CO 2 /O 2 permeation is developed by using nanoMOFs with different pore structures as gas "switches". Combined with experimental data and molecular simulation results show that the selective CO 2 /O 2 permeations of nanoMOFs/carboxymethylcellulose(CMC)/Zein are successfully controlled from 2.87 ± 0.12 to 8.65 ± 1.63 owing to the synergistic effect of nanoMOFs with different pore structures and the different affinity between nanoMOFs and molecules of CO 2 and O 2. In which, 1.6 % HKUST-1/CMC/Zein has the best CO 2 /O 2 selectivity of 8.65 ± 1.63. Furthermore, the 1.6 % HKUST-1/CMC/Zein with excellent antibacterial activity and selective CO 2 /O 2 permeation can maintain the appearance and freshness of mango for at least 7 days compared with other packaging films. Therefore, we have developed a new type of gas "switches" for MAP to accurately control the selective permeation of gases at the molecular level, which will expand the application of MAP in food preservation field. [ABSTRACT FROM AUTHOR]