The effect of promoter cobalt and the sequences of adding cobalt and molybdenum precursors on the performance of sulfur-resistant methanation were investigated. All these samples were prepared by impregnation method and characterized by N2-adsorption, X-ray diffraction(XRD), temperature-programmed reduction(TPR) and laser Raman spectroscopy(LRS). The conversions of CO for Mo-Co/Al, Co-Mo/Al and CoMo/Al catalysts were 59.7%, 54.3% and 53.9%, respectively. Among these catalysts, the Mo-Co/Al catalyst prepared stepwisely by impregnating Mo precursor firstly showed the best catalytic performance. Meanwhile, the conversions of CO were 48.9% for Mo/Al catalyst and 10.5% for Co/Al catalyst. The addition of cobalt species could improve the catalytic activity of Mo/Al catalyst. The N2-adsorption results showed that Co-Mo/Al catalyst had the smallest specific surface area among these catalysts. CoMoO4species in CoMo/Al catalyst were detected with XRD, TPR and LRS. Moreover, crystal MoS2which was reported to be less active than amorphous MoS2was found in both Co-Mo/Al and CoMo/Al catalysts. Mo-Co/Al catalyst showed the best catalytic performance as it had an appropriate surface structure, i.e., no crystal MoS2and very little CoMoO4species. Both the samples were prepared by impregnation method and characterized by N2-adsorption, X-ray diffraction (XRD), temperature- The reduction of TPR and laser Raman spectroscopy (LRS). The conversions of CO for Mo-Co / Al, Co-Mo / Al and CoMo / Al catalysts were 59.7%, 54.3% and 53.9% the addition of cobalt species could improve the Mo-Co / Al catalyst prepared by the first catalytic activity The catalytic activity of Mo / Al catalyst. The N2-adsorption results showed that Co-Mo / Al catalyst had the smallest specific surface area among these catalysts. CoMoO4species in CoMo / Al catalyst were detected with XRD, TPR and LRS. MoS2which was Mo-Co / Al catalyst showed the best catalytic performance as it had an appropriate surface structure, ie, no crystal MoS2 and very little CoMoO4 species.