We have reported that Au clusters (< 2 nm) weakly stabilized by poly(N-vinyl-2-pyrrolidone) exhibit size-specific catalysis for various types of aerobic oxidation reactions.1 These results have encouraged us to develop more robust and reusable Au cluster catalysts by immobilizing them on solid supports. However, the structural parameters, such as size, composition, and surface state must be controlled at the atomic precision in order to optimize and understand the origin of catalysis of the supported Au clusters. We have exploited a synthetic method by using ligand-protected coinage metal (Au and Ag) clusters as precursors. This talk will introduce our efforts toward atomically precise control of size,2–4 composition,5–7 and surface modification8 of the supported coinage metal clusters. Impacts of the structural parameters on catalytic performance in aerobic oxidation will be discussed.