Nickel catalysts supported on the perovskite oxide CaTiO3 (CTO) were prepared by an impregnation method for CO methanation to produce synthetic natural gas (SNG). X-Ray diffraction, nitrogen adsorption, scanning electron microscopy, transmission electron microscopy, thermogravimetric analysis, H 2-temperature programmed reduction and desorption, and X-Ray photoelectron spectroscopy were employed for the characterization of samples. The results revealed that the Ni/CTO catalysts showed a better performance than Ni/Al2O3 for CO methanation at various reaction conditions. The life time test at 600 °C and 3.0 MPa indicates that Ni/CTO is also more active, thermally stable and resistant to carbon deposition. This is because of the relatively weak Ni-CTO support interaction, highly stable CTO support, the absence of acidic sites on the surface of CTO and the proper Ni particle size of about 20-30 nm. The work is important for the development of effective methanation catalysts for SNG production.