Numerous studies of heterogeneous catalysis systems clearly demonstrate that the metal nanoparticle (NPs)/support interaction is significant in determining the catalytic chemistry. Theoretical simulations have been performed to understand the metal/support interactions [1,2]. For example, theorists discovered that electronic and oxygen defects of γ-Al2O3 anchor the active particles [1]. Platinum NPs dispersed on γ-alumina is one of the most widely used heterogeneous catalysts and Pt performs extremely well as a catalyst for the oxygen-reduction reaction used in fuel cell industries. Hence, we chose Pt/γ-Al2O3 as a model heterogeneous catalyst system to investigate the metal NPs/support interface by electron microscopy methods with the ultimate goal of bridging the gap with theoretical simulations of the interfacial atomic and electronic structure. However, theoretical simulations assume single crystal, planar supports with no impurities, but commercial γ-Al2O3 is polycrystalline and irregular in shape [3]. Hence, we are producing a model catalyst support via oxidation of single crystal NiAl to create crystalline and planar γ-Al2O3.