A mesoporous silica-coated Ni-based catalyst was developed for selective CO methanation, which is a promising candidate as a new hydrogen purification process for residential polymer electrolyte fuel cell systems. The catalytic activity and CO removal ability of the Ni/AlVOX catalyst were significantly improved by the coating of mesoporous silica on the Ni/AlVOX. The Ni-V species transported from the Ni/AlVOX to the coating layer may also act as active sites for CO methanation and thus may have an essential role in the improvement of the catalytic activity. Fe addition to the catalyst was effective for the improvement of catalyst durability due to suppression of the deposition of carbonaceous species during the reaction. (C) 2014 Elsevier B.V. All rights reserved.