An Al2O3-ZrO2 support was prepared by grafting a zirconium precursor onto the surface of commercial γ-Al2O3. A physical mixture of Al2O3-ZrO2 was also prepared for the purpose of comparison. Ni/Al2O3-ZrO2 catalysts were then prepared by an impregnation method, and were applied to the hydrogen production by steam reforming of liquefied natural gas (LNG). The effect ZrO2 and preparation method of Al2O3-ZrO2 on the performance of supported nickel catalysts in the steam reforming of LNG was investigated. The Al2O3-ZrO2 prepared by a grafting method was more efficient as a support for nickel catalyst than the physical mixture of Al2O3-ZrO2 in the hydrogen production by steam reforming of LNG. The well-developed tetragonal phase of ZrO2 and the high dispersion of ZrO2 on the surface of γ-Al2O3 were responsible for the enhanced catalytic performance of Ni/Al2O3-ZrO2 prepared by way of a grafting method.