In this research, xylene was utilized as a simulated gas, γ-Al2O3 pellets were selected as catalyst carriers, and FeOx, MnOx, CeOx, and CuOx were used as active components to analyze the synergistic treatment of VOCs-O3 by low-temperature plasma combined with supported catalysts. Different metal oxides and other factors influence the synergistic treatment of VOCs-O3. The results showed that the catalytic effect of Fe-Mn/γ-Al2O3 prepared by the equivalent volumes of consecutive impregnation method was better than that of Fe-Mn/γ-Al2O3 prepared by co-impregnation method. When combined with low temperature plasma technology, high-energy electron collision reaction and oxidation reaction between free radicals occurs, which played a synergistic role in the degradation of VOCs-O3. The total removal rate of xylene was 94.88%, and the depletion rate of ozone was 84.1%.