Through the weak and non-covalent interactions of peptides with inorganic nanomaterials, selective and responsive biointerfaces are possible that are prohibited by the strong covalent binding of standard ligands that locks the molecules into a single configuration. Unfortunately, biomolecules are not typically responsive to external stimuli to trigger molecular reconfiguration, thus modification of the structure is required. By merging a peptide with known affinity for Au with a non-biological photoactuatable molecule, azobenzene, stimuli-responsive nanoparticle biointerfaces have been realized. The hybrid biomolecule maintains substantial affinity for Au; however, its biomolecular configuration on a nanoparticle can been reversibly reconfigured via azobenzene isomerization based upon photo-illumination without destabilizing the nanoparticle. Interestingly, the photoisomerization rate, and thus biomolecular reconfiguration, is highly dependent upon the inorganic composition. These results pave the way toward controllable and reconfigurable nanoparticle biomolecular interfaces to engender a single nanosystem with multiple functionalities/properties that are independently and selectively enabled.