Bimetallic catalysts provide the ability to tune catalytic activity, selectivity, and stability. Model catalysts with size-selected bimetallic clusters on well-defined supports offer a useful platform for studying catalytic mechanisms, however, producing size-selected bimetallic clusters can be challenging. In this study, we present a way to prepare bimetallic model (Pt n B m /alumina) cluster catalysts by depositing size-selected Pt 7 clusters on an alumina thin film, then selectively adding boron by exposure to diborane and heating. The interactions between Pt 7 /alumina and diborane were probed using temperature-programmed desorption/reaction (TPD/R), X-ray photoelectron spectroscopy (XPS), low energy ion scattering (ISS), plane wave density functional theory (PW-DFT), and molecular dynamic (MD) simulations. It was found that the diborane exposure/heating process does result in preferential binding of B in association with the Pt clusters. Borated Pt clusters are of interest because they are known to exhibit reduced affinity to carbon deposition 1 in catalytic dehydrogenation. At high temperatures, theory, in agreement with experiment, shows that boron tends to migrate to sites beneath the Pt clusters forming Pt-B-O suf bonds that anchor the clusters to the alumina support.