The efficiency of gas separation by mixed-matrix membranes (MMMs) derived from poly(4-methyl-1-pentene) (PMP) filled by zinc oxide nanoparticles is investigated. The membranes are prepared by the solvent evaporation method. The zinc oxide nanoparticles are loaded at different weight percentages. The results reveal that adding zinc oxide nanoparticles at all loading percentages of the nanoparticles increases the selectivity of all gas pairs such as O2/N2, CO2/CH4, and CO2/N2. Furthermore, the CO2 permeability in PMP-zinc oxide MMMs was significantly improved when increasing the feed pressure.