Plant photosynthetic machinery is the main source of acquisition and conversion of solar energy to chemical energy with the capacity for autonomous self-repair. However, the major limitation of the chloroplast photosystem is that it can absorb light only within the visible range of the spectrum, which is roughly 50% of the incident solar radiation. Moreover, the photosynthetic apparatus is saturated by less than 10% of available sunlight. If the capacity of solar light absorption and the transmission of resulting photons through the photosynthetic electron transport chain (ETC) can be extended, the overall efficiency of photosynthesis can be improved. The plant nanobionic approach can address this via the introduction of nanoparticles into or in the vicinity of the photosynthetic machinery/chloroplast. We have studied this exceptional nanobionic-mediated capability of two optically active nanostructures and evaluated the impact of their optical properties on plant photosynthesis. Our study revealed that metal (Ag) and core-shell metal nanostructures (AgS) can increase light absorption and improve electron transport through ETC. Both nanostructures were found to have a beneficial effect on the photoluminescence property of the isolated chloroplast. Translocation studies confirmed systemic transportation of the nanomaterial in different plant tissues. The primary growth parameters showed no detrimental effect until 21 days of treatment on . The nano silver/silica core/shell structure (AgS) was found to be more advantageous over nano silver (AgNP) in photon entrapment, light-dependent biochemical reactions, and toxicity parameters. In the future, these nanostructures can enhance photosynthesis by increasing light absorption and resulting in higher assimilatory power generation in the form of ATP and NADPH. This approach may lead to a paradigm shift toward a sustainable method for the configuration of plant chloroplast-based hybrid energy harvesting devices.