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Abstract Engineering the nucleation and growth of plasmonic metals (Ag and Au) on their pre‐existing seeds is expected to produce nanostructures with unconventional morphologies and plasmonic properties that may find unique applications in sensing, catalysis, and broadband energy harvesting. Typical seed‐mediated growth processes take advantage of the perfect lattice match between the deposited metal and seeds to induce conformal coating, leading to either simple size increases (e.g., Au on Au) or the formation of core–shell structures (e.g., Ag on Au) with limited morphology change. In this work, we show that the introduction of a thin layer of metal with considerable lattice mismatch can effectively induce the nucleation of well‐defined Au islands on Au nanocrystal seeds. By controlling the interfacial energy between the seed and the deposited material, the oxidative ripening, and the surface diffusion of metal precursors, we can regulate the number of islands on the seeds and produce complex Au nanostructures with morphologies tunable from core‐satellites to tetramers, trimers, and dimers.