Metal clusters typically consist of two to a few hundred atoms and have unique properties that change with the type and number of atoms that form the cluster. Metal clusters can be generated with a precise number of atoms, and therefore have specific size, shape, and electronic structures. When metal clusters are deposited onto a substrate, their shape and electronic structure depend on the interaction with the substrate surface and thus depend on the properties of both the clusters and those of the substrate. Deposited metal clusters have discrete, individual electron energy levels that differ from the electron energy levels in the constituting individual atoms, isolated clusters, and the respective bulk material. The properties of clusters with a focus on Au and Ru, the methods to generate metal clusters, and the methods of deposition of clusters onto substrate surfaces are covered. The properties of cluster‐modified surfaces are important for their application. The main application covered here is catalysis, and the methods for characterization of the cluster‐modified surfaces are described.