To obviously reduce the sintering behavior of Ni particles in Ni/α-Al₂O₃ catalysts during CO methanation reaction, ZrO₂ was deposited onto the Ni/α-Al₂O₃ catalyst surface by a modified impregnation method. It was observed that the ZrO₂-modified catalyst with an appropriate amount of ZrO₂ showed enhanced catalytic activity due to the increased H₂ uptake and Ni dispersion. During the 103h-lifetime test, the ZrO₂-modified catalyst exhibited higher stability and anti-sintering performance than the unmodified one, because the partial coverage of ZrO₂ particles could effectively prevent Ni particles from sintering during the reaction at high temperatures. The findings obtained in this study should be conducive to the design and development of supported metal catalysts for high temperature reactions with enhanced stability.