Abstract: Ni-Fe/montmorillonite (MMT) catalysts were prepared by impregnation method for hydrogen production via ethanol steam reforming. The catalysts were characterized by XRD, H₂-TPR, and N₂ adsorption-desorption. It was found that Ni-Fe bimetallic catalysts exhibited higher activities and stability than single metallic catalysts due to the well dispersed Ni-Fe, small nickel crystallites and stronger interaction between Ni²⁺ and carrier. The conversion and selectivity were affected by the ratio of Ni to Fe. The 10Ni5Fe/MMT catalyst showed the optimum catalytic performance, its ethanol conversion was 100%, the selectivity of hydrogen gas remained at 72%, and selectivity of CO and CH₄ were significantly decreased at 500℃ during 30h testing. This could be attributed to the promoter Fe, which improves the dispersion of Ni and results in a good ESR activity at low reaction temperature. Small Ni particles can suppress methane formation and Fe addition can enhance the methane reforming with water and water gas shift reaction, resulting in higher selectivity of hydrogen.