The growth of Ag on a graphite surface decorated by size selected Au “seed” nanoclusters is investigated. Compared with the behavior on bare graphite, the deposition of the Au clusters decreases the lateral diffusion of Ag atoms and enables the growth of Ag/Au nanostructures on/ around the top of the initial Au clusters. Depending on the Au cluster shape, which can be tuned by the cluster deposition energy, Ag deposition either leads to 2 ML high platelets or three-dimensional nanoclusters. This cluster seeding technique shows potential for the rapid production of binary model catalysts, biochips, and optical films