A mesoporous Ni-Al2O3-ZrO2 aerogel (Ni-AZ) catalyst was prepared by a single-step epoxide-driven sol-gel method and a subsequent supercritical CO2 drying method. For comparison, a mesoporous Al2O3-ZrO2 aerogel (AZ) support was prepared by a single-step epoxide-driven sol gel method, and subsequently, a mesoporous Ni/Al2O3-ZrO2 aerogel (Ni/AZ) catalyst was prepared by an incipient wetness impregnation method. The effect of preparation method on the physicochemical properties and catalytic activities of Ni-AZ and Ni/AZ catalysts was investigated. Although both catalysts retained a mesoporous structure, Ni/AZ catalyst showed lower surface area than Ni-AZ catalyst. From TPR, XRD, and H-2-TPD results, it was revealed that Ni-AZ catalyst retained higher reducibility and higher nickel dispersion than Ni/AZ catalyst. In the hydrogen production by steam reforming of ethanol, both catalysts showed a stable catalytic performance with complete conversion of ethanol. However, Ni-AZ catalyst showed higher hydrogen yield than Ni/AZ catalyst. Superior textural properties, high reducibility, and high nickel surface area of Ni-AZ catalyst were responsible for its enhanced catalytic performance in the steam reforming of ethanol. Copyright (C) 2013, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.