The influence of the substrate on the morphology of 2D and 3D superlattices made of 5.8 nm silver sulfidenanocrystals coated with dodecanethiol is reported. The two substrates used are highly oriented pyrolyticgraphite (HOPG) and molybdenum disulfide (MoS2). The self-assemblies of nanocrystals were characterizedwith scanning electron microscopy and atomic force microscopy techniques, and it was found that theself-organization in 2D and 3D superlattices markedly differs with the substrate used. These changes inbehavior are explained in terms of particle−particle and particle−substrate van der Waals interactionsand capillary forces.