The　Ni-Mo　catalyst　has　attracted　significant　attention　due　to　its　excellent　coke-resistance　in　dry　reforming　of　methane　(DRM)　reaction,　but　its　detailed　mechanism　is　still　vague.　Herein,　Mo-doped　Ni　(Ni-Mo-x)　and　MoOx　adsorbed　Ni　surfaces　(MoOx@Ni)　are　employed　to　explore　the　DRM　reaction　mechanism　and　the　effect　of　coke-resistance.　Due　to　the　electron　donor　effect　of　Mo,　the　antibonding　states　below　the　Fermi　level　between　Ni　and　C　increase　and　the　adsorption　of　C　decrease,　thereby　inhibiting　the　carbonization　of　Ni.　On　account　of　the　strong　Mo　and　O　interaction,　more　O　atoms　gather　around　Mo,　which　inhibits　the　oxidation　of　Ni　and　may　promote　the　formation　of　MoOx　species　on　the　Ni-Mo　catalyst.　The　presence　of　Mo-O　species　promotes　the　carbon　oxidation,　forming　a　unique　redox　cycle　(MoOx　＜-＞　MoOx-1)　similar　to　the　Mars-van　Krevelen　(MvK)　mechanism,　explaining　the　excellent　anti-carbon　deposition　effect　on　the　Ni-Mo　catalyst.