Arsenic species, which are inevitable components in flue gas from the coal combustion process, will result in severe deactivation of selective catalytic reduction (SCR) catalysts. In this paper, a novel method is proposed to regenerate the arsenic-poisoned commercial V2O5-MoO3/TiO2 catalyst collected from coal-fired power plants, including ammonia washing, H2 reduction, and air calcination. Activity tests indicated that the proposed method could recover the catalyst activity more than 96% of the fresh catalyst. Furthermore, detailed characterizations results indicated that this regeneration method could not only effectively remove the arsenic species, but also recover the active constituents of the catalysts to a considerable level. The proposed method offers a feasible strategy for the regeneration of poisoned commercial SCR catalysts and can effectively reduce the total denitrification cost for coal-fired power plants.