Mesoporous nanocrystalline cerium(IV) oxide (CeO2) with high surface area was synthesized by precipitation using a cationic surfactant and employed as support for a nickel catalyst in CO methanation. The preparation factors of CeO2 were optimized by the Taguchi method to achieve a sample with high surface area. The obtained results reveal that the sample prepared under optimized conditions has a mesoporous structure with high surface area and crystallite size. The addition of a surfactant significantly influences the structural properties of CeO2 and improves the specific surface area. The optimized sample was employed as support for a nickel catalyst in CO methanation reaction. The prepared catalyst possessed a high activity compared to a commercial methanation catalyst.