Novel heterostructured nanoparticles were synthesized by the deposition of Ag on Pt nanocubes by overcoming lattice mismatch, where Ag deposition preferentially occurred at corners of Pt nanocubes during the initial stage of deposition, and position and amount of Ag deposition were controlled by tuning of reaction conditions. The mechanism of such site-specific deposition of Ag is discussed in relation to I- (shape forming agent) and succinate (organic protective agent).