Theeffectofpromotercobaltandthesequencesofaddingcobaltandmolybdenumprecursorsontheperformanceofsulfur-resistantmethanationwereinvestigated.AllthesesampleswerepreparedbyimpregnationmethodandcharacterizedbyN2-adsorption,X-raydiffraction(XRD),temperature-programmedreduction(TPR)andlaserRamanspectroscopy(LRS).TheconversionsofCOforMo-Co/Al,Co-Mo/AlandCoMo/Alcatalystswere59.7%,54.3%and53.9%,respectively.Amongthesecatalysts,theMo-Co/AlcatalystpreparedstepwiselybyimpregnatingMoprecursorfirstlyshowedthebestcatalyticperformance.Meanwhile,theconversionsofCOwere48.9%forMo/Alcatalystand10.5%forCo/Alcatalyst.TheadditionofcobaltspeciescouldimprovethecatalyticactivityofMo/Alcatalyst.TheN2-adsorptionresultsshowedthatCo-Mo/Alcatalysthadthesmallestspecificsurfaceareaamongthesecatalysts.CoMoO4speciesinCoMo/AlcatalystweredetectedwithXRD,TPRandLRS.Moreover,crystalMoS2whichwasreportedtobelessactivethanamorphousMoS2wasfoundinbothCo-Mo/AlandCoMo/Alcatalysts.Mo-Co/Alcatalystshowedthebestcatalyticperformanceasithadanappropriatesurfacestructure,i.e.,nocrystalMoS2andverylittleCoMoO4species.