An in-depth understanding of the influence mechanism of the nonprecious metal Fe promoter on CO 2 methanation is of great significance to the optimal design of high-efficiency CO 2 methanation catalysts. In this research, CeO 2 and Al 2 O 3 -supported Ni-based catalysts were prepared and evaluated for the CO 2 methanation reaction. Interestingly, it was found that the addition of Fe into the CeO 2 -supported Ni catalyst lowered the CO 2 methanation performance, while it greatly enhanced the performance of the Al 2 O 3 -supported Ni catalyst. A variety of factors over Fe-modified catalysts were explored, in which surface basicity along with oxygen vacancies could contribute to the adjustment of the CO 2 methanation performance.