Catalysts created by loading FeOx and AgOx on SBA-15 surfaces via wet impregnation were used to remove toluene with the assistance of non-thermal plasma (NTP). The catalysts were characterized with X-ray diffraction (XRD), scanning electron microscopy (SEM), and H2 temperature-programmed reduction (H2-TPR). The results showed that incorporating the SBA-15, 3%FeOx/SBA-15 and 2%FeOx–1%AgOy/SBA-15 catalysts enhanced the toluene removal efficiency and CO2 selectivity of the NTP system. The silver particles tended to cover the catalyst surface in the form of Ag and Ag2O, which lengthened the residual time of toluene in the NTP-catalytic system, thereby promoting the reaction of toluene with oxygen on the catalyst surface. Simultaneously, introducing Ag improved the distribution of FeOx on the catalyst surface, increasing toluene oxidation and catalyst stability. According to our analysis of the toluene removal efficiency, identification of organic byproducts, and in situ FT-IR spectroscopy of the toluene adsorption, FeOx and AgOx significantly enhance the efficiency of toluene degradation in plasma-assisted catalytic systems.