Harvesting solar energy for chemical transformations is gaining a rising interest in promoting the clean and modular chemical synthesis approach and addressing conventional thermocatalytic systems’ limitations. Under light irradiation, noble metal nanoparticles, particularly those characterized by localized surface plasmon resonance, commonly known as plasmonic nanoparticles, generate a strong electromagnetic field, excited hot carriers, and photothermal heating. The catalytic activity of Plasmonic nanoparticles can be enhanced by incorporating transition metal catalysts as co-catalysts, promoters or stabilizers. In this talk, we demonstrate that by modifying the atomic structure of hybrid plasmonic nanocatalysts via femtosecond pulsed laser we are able to not only enhance the optoelectronic and catalytic properties of the resulting nanoparticles, but also to improve the mechanical stability of these hybrid nanostructures, which are of paramount importance for industrial applications. We also investigate the trade-off between the effect of light absorption, catalytic activity, and mechanical stability by optimizing the structure and composition of hybrid plasmonic nanoparticles. This work provides insight into the design of hybrid plasmonic-catalytic nanostructures with improved performance and stability for solar-fuel-based applications.