A mesoporous Ni-Al2O3 aerogel catalyst was prepared by a single-step epoxide-driven sol-gel method and a subsequent supercritical CO2 drying method (NA-ES catalyst). For comparison, a mesoporous Ni-Al2O3 aerogel catalyst was also prepared by a single-step alkoxide-based sol-gel method and a subsequent supercritical CO2 drying method (NAAS catalyst). Differences in physicochemical properties and catalytic activities of mesoporous Ni-Al2O3 aerogel catalysts in the steam reforming of liquefied natural gas (LNG) were investigated. Textural properties of Ni-Al2O3 aerogel catalysts were affected by the preparation method. Nickel species were highly dispersed in alumina through the formation of nickel aluminate phase in both NA-ES and NA-AS catalysts. However, chemical states of Al atoms in both catalysts were quite different. In addition, nickel species in the NA-ES catalyst exhibited high reducibility and high dispersion compared to those in the NA-AS catalyst. In the steam reforming of LNG, NA-ES catalyst exhibited a better catalytic performance than NA-AS catalyst in terms of LNG conversion and hydrogen yield, although both catalysts showed a stable catalytic performance during the reaction without deactivation behavior. Furthermore, NA-ES catalyst with small average nickel diameter suppressed water-gas shift reaction. Reducibility and dispersion of nickel species served as important factors determining the catalytic performance of the catalysts. Copyright (C) 2011, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.