V2O5-WO3(MoO3)/TiO2 catalysts have been widely used for NOX removal owing to their excellent catalytic performance; however, they suffer from a narrow operating temperature range, reduced N-2 selectivity at a high temperature, and deteriorated activity due to SO2 poisoning. In this study, a phase-controlled 1T/2H-MoS2 was prepared by a one-step hydrothermal method and used as a Mo precursor to develop V-Mo/Ti catalysts with improved selective catalytic reduction (SCR) performance. Raman analysis confirmed that the heterogeneous MoS2 contains a partially formed 1T phase, which facilitated the generation of active sites in the catalyst. The heterogeneous 1T/2H-MoS2 also produced a considerable amount of surface oxygen species on the V-Mo/Ti catalyst, which increased the V4+/(V4++V5+) ratio. The resulting catalyst maintained a NOX conversion of over 96% from 250 degrees C to 400 degrees C and demonstrated excellent N-2 selectivity and resistance to SO2 poisoning.