A superior desulfurization catalyst (AC-Cop) was synthesized by blending copper ore and coals through a one-step carbonization activation process. The sulfur capacities of the modified catalysts were enhanced significantly and that of AC-Cop with 1 wt % of copper ore was 174.8 mg/g which was 50% higher than that of blank activated coke. Their excellent desulfurization performance could be attributed to the introduction of much more active sites on the surface of AC-Cop, i.e., CuO, Fe2O3, Fe3O4, and C=O groups, which promoted the adsorption and oxidation of SO2. In addition, the used AC-Cop could be easily regenerated by thermal treatment, with a slow decrease in desulfurization performance during four desulfurization regeneration cycles. This was ascribed to the gradual accumulation of the desulfurization products, i.e., Fe-2(SO4)(3) and CuSO4 and the decreased contents of C=O groups. The results suggested that such copper ore-modified activated coke could be a kind of efficient, regenerable, and inexpensive desulfurization catalyst.