Economic membrane technologies are a perennial hot topic in the field of natural gas purification and O2 enrichment. In this work, novel hyper cross-linked polymers (HCPs) incorporating 6-FDA based polyimide (PI) MMMs were prepared via a casting method for enhancing different gas transport (CO2, CH4, O2, and N2). The gas permeation experiments showed that compared with pure PI films, adding HCPs effectively promotes gas transport, increases gas permeability, and maintains ideal selectivity. The permeability of HCPs/PI MMMs toward CO2 and O2 was as high as 105.85 barrer and 24.03 barrer, respectively, and the ideal selectivity of CO2/CH4 and O2/N2 was 15.67 and 3.00, respectively. Molecular dynamic simulations further verified that adding HCPs was beneficial to gas transport thanks to large FFV of MMMs. Thus, HCPs have potential utility in the fabrication of MMMs for facilitating gas transport in the field of natural gas purification and O2 enrichment.