Herein, we report the successful application of hybrid Au-Ag nanoparticles (NPs) and nanochains (NCs) in the harvesting, of visible light energy for selective hydrogenation reactions. For individual Au@Ag NPs with Au25 cores, the conversion and turnover frequency (TOP) are approximately 8 and 10 times higher than those of Au25 NPs, respectively. Notably, after the self-assembly of the Au@Ag NPs, the conversion and TOF of 1D NCs were approximately 2.5 and 2 times higher than those of isolated Au@Ag NPs, respectively, owing to the coupling of surface plasmon and the increase in the rate at which hot (energetic) electrons are generated with the formation of plasmonic hot spots between NPs. Furthermore, the surface-enhanced Raman scattering (SERS) activity of 1D Au@Ag NCs was strengthened by nearly 2 orders of magnitude.