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Materials that intrinsically exhibit localized surface plasmon resonance (LSPR) in the visible region have been predominantly researched on nanoparticles (NPs) composed of coinage metals, namely Au, Ag, and Cu. Here, as a coinage metal‐free intermetallic NPs, colloidal PtIn2 NPs with a C1 (CaF2‐type) crystal structure are synthesized by the liquid phase method, which evidently exhibit LSPR at wavelengths similar to face‐centered cubic (fcc)‐Au NPs. Computational simulations pointed out differences in the electronic structure and photo‐excited electron dynamics between C1‐PtIn2 and fcc‐Au NPs; reduces interband transition and stronger screening with smaller number of bound d‐electrons compare with fcc‐Au are unique origins of the visible plasmonic nature of C1‐PtIn2 NPs. These results strongly indicate that the intermetallic NPs are expected to address the development of alternative plasmonic materials by tuning their crystal structure and composition. [ABSTRACT FROM AUTHOR]