Promoter-modified Ni-based catalysts were synthesized by an incipient-wetness impregnation method using 3D-mesoporous KIT-6 as a support modified by ethylene glycol, and evaluated for the catalytic production of synthetic natural gas (SNG) from CO methanation. Characterization results suggested that the addition of promoter species could remarkably improve the low-temperature catalytic activity for CO methanation, which was due to a large dispersion of Ni nanoparticles, an enhanced interaction between metal and support as well as a confinement effect of 3D-mesopores. Among all catalysts, Ni-V/KIT-6 possessed the best catalytic performance, which was ascribed to the largest H2 uptake of 177.6 ^mol/g and Ni dispersion of 26.5%, an intimate interaction with the support from the formation of Si-O-V linkage and an enhanced confinement effect of 3D-mesopores to effectively prevent the growth of Ni nanoparticles and carbon filaments. In consequence, Ni-V/KIT-6 displayed excellent catalytic performance as well as high catalytic stability, which can be regarded as a promising candidate for CO methanation.