A strong enhancement of electromagnetic field generated through resonating surface polaritons on metal films and particles has stimulated considerable interest in diverse research fields such as photobiology as, for example, in photosynthesis. This surface plasmon resonance (SPR) of metal nanoparticles (NPs) can augment photosynthetic chemical energy production in an artificial photosynthetic model system. In this paper, the effect of three water-dispersible gold NPs (GNPs) of nearly similar size but with different surface moieties (aspartate, bovine serum albumin, and citrate capping) is experimentally shown on the photosynthetic efficiency of isolated chloroplasts of Vigna radiata. It was found that GNPs can augment photon absorption in the light-harvesting molecular complexes (LHMCs) and can cause increased distinctive optical and electronic properties. Photosynthetic light reactions like electron transport rate, photophosphorylation, and oxygen evolution rate were increased in the presence of GNPs, indicating higher photosynthetic activity. The rate of increase was dependent on the surface capping of GNPs, and it was maximum in case of citrate-capped GNP. Moreover, it was also found that these GNP-induced enhancements had positive correlation with the primary growth parameters of V. radiata.