Hydrogenolysis and dehydrogenation of propane were studied over model nickel-gold catalysts. The supported model Ni-Au catalysts were prepared by depositing Ni and Au onto a planar silica film. Infrared reflection absorption spectroscopic data showed that isolated Ni sites appeared and became dominant on the surface with the addition of Au to Ni. For the conversion of propane in the presence of hydrogen, the dehydrogenation of propane to propylene was observed on the Ni-Au bimetallic catalysts, whereas only hydrogenolysis products were observed on the monometallic Ni catalyst. A correlation was found between the concentration of isolated Ni sites and the catalytic activity for propane dehydrogenation.