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Toluene, as a kind of volatile organic compounds, not only causes pollution to the atmosphere and water but also damages human health. Although vacuum ultraviolet (VUV) can effectively promote the degradation of toluene, it will produce a large amount of O 3 , which will cause secondary pollution. Therefore, it is very important to study catalysts that can promote both toluene degradation and ozone decomposition. In this work, a MnO 2 /TiO 2 catalyst with uniformly dispersed MnO 2 was prepared using the immersion reduction method, which was used to degrade toluene under VUV. The toluene removal efficiency was improved by the utilization and elimination of O 3 . The toluene removal efficiency over the prepared MnO 2 /TiO 2 catalyst was 88%, and the O 3 removal rate was 97%. The toluene removal efficiency under VUV was 4.9 times that of UV. The synergistic effect of VUV and multifunctional catalyst effectively improved the toluene removal efficiency.