Catalytic generation of hydrogen by partial oxidation of ethanol over a series of Ni-Fe catalysts has been studied. The catalytic performances have been investigated under various O-2 and C2H5OH molar ratios at 473-573 K. These Ni-Fe catalysts showed high activities for the partial oxidation of ethanol to hydrogen. The rate of hydrogen generation increased with the increase of temperature. Among the different Ni-Fe catalysts, Ni(5)0Fe(5)0 had the best activity. The conversion of ethanol reaches 86.91% and selectivity to hydrogen reaches 46.23% at optimum reaction conditions, i.e., O-2/C2H5OH =1.5, T=573 K. XRD patterns of the catalysts showed that their main components are spinal-type magnetite and FeNi3 alloy. XPS results indicated that the bulk of catalyst is mainly FeNi3 alloy and the surface is mainly magnetite. The possible mechanism has been discussed.