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Localized surface plasmon resonances (LSPRs) in heavily doped copper chalcogenides are unique because LSPR energy can be adjusted by adjusting doping or stoichiometry. However, there are few investigations on the LSPRs of bimetal copper-based chalcogenides. Herein, bimetal Cu5FeS4 (CFS) nanoparticles were synthesized by a facile hot injection of a molecular precursor. The tunable plasmon resonance absorption of CFS nanoparticles is achieved by the decrease of the ratio of copper to iron and the treatment of n-dodecylphosphoric acid (DDPA