New bimetallic Ni-Au supported nanoparticle catalysts were prepared by using dendrimer templated nanoparticles. Amine-terminated generation 5 polyamidoamine (PAMAM) dendrimers were anchored to a commercial silica with a siloxane linked anhydride. The dendrimer was then alkylated and used to template Ni-Au nanoparticles, which were subsequently extracted into organic solution as thiol monolayer protected clusters (MPCs). Transmission electron microscopy (TEM) and energy dispersive spectroscopy (EDS) indicated bimetallic nanoparticles of about 2 nm in size. Nanoparticles were deposited onto P-25 TiO2, and the capping thiol ligands were removed under flowing H2. DRIFTS infrared spectra of adsorbed CO showed only Au on the catalyst surface; no bands attributable to Ni or NiO were observed. Density functional theory (DFT) calculations showed that Au is substantially more stable than Ni on the surface of model slabs. DFT calculations also indicated that the incorporation of Ni into Au slabs results in stronger adsorption of O and CO on Au surfaces. Catalysts were evaluated with low-temperature CO oxidation. Kinetics studies indicated a substantial modification of Au catalysis through Ni incorporation. Apparent activation energies decreased by more than 50% and O2 reaction orders increased from 0.2 to 0.9. These results are placed in the context of the available literature regarding support effects for Au catalysts. The observed changes to Au chemistry in the current work are substantially larger than previous reports have attributed to support effects. A Michaelis-Menten (enzyme) treatment of the kinetics data indicated that the O2 reactivity constant increased by a factor of 40 for catalysts with high Ni content. This was in good qualitative agreement with the DFT calculations. At the same time, the introduction of Ni reduced the relative number of catalytically active sites.