Iron-doped LaNiO3 catalysts with a perovskite structure were prepared via self-combustion and tested in auto-thermal reforming (ATR) of ethanol. Characterizations of temperature-programmed surface reaction (TPSR), X-ray diffraction (XRD), physical N-2 adsorption, and temperature-programmed reduction (TPR) were carried out. The results indicate that LaNiO3 perovskite structure was successfully formed via self-combustion. With iron-doping in LaNiO3, the perovskite structure still remains, in the form of solid solution La(Ni, Fe)O-3, where iron is reducible and the nickel-iron alloy forms after the reduction. In addition, the surface area of the iron-doped samples increased. The TPSR results indicate that with iron-doping, the activity for adsorbed ethanol species is modified and a higher activity for methane transformation is achieved. As a result, an LNE10 sample (LaNi0.90Fe0.10O3) with both nickel and nickel-iron alloy shows better performance in ATR: the ethanol conversion is near 100%, while the selectivity to by-products, such as ethylene, ethane, acetaldehyde and methane, is decreased, and CO2 is the main carbon-containing product; consequently, a hydrogen yield near 3.0 mol H-2/mol EtOH is obtained and remains stable in the 30-h test of ATR. Copyright (C) 2011, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.