Converting coal-based gas to natural gas has great economic and environmental benefits. As coal gasification technology matures, the CO methanation process acts as an important role. MOFs materials have shown excellent performance in many fields and have attracted more and more attention. Compared with conventional catalysts, UiO-66 is a Zr-based MOFs material with high specific surface area and good thermal and chemical stability, the active metal Ni has low cost and is equivalent to the catalytic hydrogenation ability of precious metals. In present study, a series of UiO-66 catalysts with Ni loading were prepared via ultrasonic impregnation method. Plenty of characterizations including XRD, BET, TG, SEM, TEM and XPS were used to study the structure, textual properties, thermal stability and morphology of the UiO-66 supported Ni-based catalysts. The catalytic performance of different catalysts was also evaluated in the fixed-bed reactor. The results showed that the Ni was reduced to metallic state in the prepared catalyst, the Ni metal was highly dispersed on the UiO-66 support and exhibited no significant effect on the framework structure and crystal morphology of the MOF material. The structure of the carrier did not change below 400℃. In the CO methanation reaction, the activation temperature of the Ni/UiO-66 catalysts gradually decreased with the increase of Ni loading content. At the same reaction temperature (320℃), the Ni content on different catalysts increased from 10% to 30%, the CO conversion increased from 10.7% to 89.7%.When the Ni content was 20%, the catalyst showed good stability during the reaction process. Meanwhile, the CO conversion on the Ni-based catalyst was much higher than that of the Fe-based and Co-based catalysts with the same metal content, indicating that Ni as an active metal had excellent catalytic performance in the synthesis gas to methane reaction process.