Formation of Au, Pt, and bimetallic Au-Pt nanostructures by thermal dewetting of single-layer Au, Pt and bilayer Au-Pt thin films on Si substrates was systematically studied. The solid-state dewetting of both single-layer and bilayer metallic films was shown to go through heterogeneous void initiation followed by void growth via capillary agglomeration. For the single-layer of Au and Pt films, the void growth started at a temperature right above the Hüttig temperature, at which the atoms at the surface or at defects become mobile. Uniformly distributed Au (7 ± 1 nm to 33 ± 8 nm) and Pt (7 ± 1 nm) NPs with monodispersed size distributions were produced from complete dewetting achieved for thinner 1.7−5.5 nm-thick Au and 1.4 nm-thick Pt films, respectively. The NP size is strongly dependent on the initial thin film thickness, but less so on temperature and time. Thermal dewetting of Au-Pt bilayer films resulted in partial dewetting only, forming isolated nano-islands or large particles, regardless of sputtering order and total thin film thickness. The increased resistance to thermal dewetting shown in the Au-Pt bilayer films as compared to the individual Au or Pt layer is a reflection of the stabilizing effect that occurs upon adding Pt to Au in the bimetallic system. Energy dispersive X-ray spectroscopic analysis showed that the two metals in the bilayer films broke up together instead of dewetting individually. According to the X-ray diffraction analysis, the produced Au-Pt nanostructures are phase-segregated, consisting of an Au-rich phase and a Pt-rich phase.