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Bio-inspired approaches for materials synthesis and application are emerging as potentially sustainable approaches to achieve functional structures with selectively controlled properties (e.g., turn on catalysis). An attractive avenue to allow for selective functionality is optical stimulation; however, the ability to make nanomaterials light responsive for many applications remains challenging. One approach is to incorporate photoswitches into the surface adsorbed ligands which can stimulate a surface structural change that could have implications on the catalytic reactivity driven by the underlying metallic nanoparticle component. Herein were demonstrate the ability to drive optical switching of surface ligand overlayer structures on peptide-capped Pt nanoparticles. To this end, incorporation of an azobenzene unit into the surface-adsorbed peptide allows for the ability to optical reconfigure the ligand overlayer structure. This change results in direct manipulation of the catalytic properties of the Pt materials for olefin hydrogenation, which demonstrated changes in reactivity not only between different reagents, but also between the different ligand structures. Such results present information which could be used in the design of ligand interface structures to trigger specific reactivity control for a variety of reactions and materials for sustainable catalysis.