Ni-based halloysite methanation catalysts with various Mo contents were prepared by using halloysites as supports, and it was used to catalyze the methanation reaction. The addition of Mo can strengthen the interaction between Ni and the halloysite, preventing the active component Ni from aggregating into the larger particles during the reaction, which can improve the catalyst activity and life. At the same time, the electron donation of the Mo atom can rise the electron density around the nickel atom and facilitate the dissociation of carbon monoxide on the Ni surface, which can improve the activity of the reaction under low temperature. Among them, the 6Mo10Ni/eHNTs catalyst has the best activity at 350 °C. The conversion of CO achieves 100% and the yield of CH 4 reaches 99.7%. At 300 °C, the CO conversion rate is 100%, and the CH 4 yield is 97%, which is the same as the activity of 10Ni/eHNTs without Mo at 350 °C, i.e., the low temperature activity is improved with the addition of Mo. At the same time, the addition of Mo enhances the anti-sintering property and resistance to the carbon deposition of the catalysts. This work shows the possibility for the industrial application of the methanation catalyst using halloysites as the support.