We investigated the interaction between polyynes (linear carbon chains) and various metal nanoparticles (Ag, Au, and Cu) to provide insight into the optical properties of metal-polyynes systems prepared by different experimental techniques. Polyynes were produced by laser ablation in deionized water, metal nanoparticles solutions, and copper chloride solution. Metal nanoparticles complexes with polyynes were analyzed by Raman, surface-enhanced Raman scattering, and UV-vis spectroscopy.