- 2017, The Minerals, Metals & Materials Society. Liquid metal dealloying is a promising route for making metal nanocomposites with a wide range of microstructure morphologies. However, it is not well suited for synthesizing nanocomposites in thin-film form. We propose a new route to fabricating fully dense nanocomposite thin films by dealloying a binary parent alloy in a unary solid metal solvent. We fabricated and tested three thin-film diffusion couples to understand the alloy design criteria for synthesizing dealloyed thin films free of cracks and voids. We find that the best-quality dealloyed thin films may be obtained from alloys that do not undergo large volume changes upon dealloying and that exhibit minimal net vacancy flux during interdiffusion.