The design of active nanostructures whose form and properties can be modulated by remote means is an important challenge in nanoscience. Here we report two types of active nanoparticle complexes, with properties controlled by near-infrared illumination, resulting from the assembly of photothermally responsive plasmonic nanoparticles with thermally labile biomolecular linkers. Au nanoshells (NS) and quantum dots (QD) are assembled using coiled-coil peptides into NS-NS and NS-QD complexes. Illumination of the NS-NS complexes results in reversible disassembly reassembly, while illumination of NS-QD complexes results in a large, reproducible modulation of the quantum dot fluorescence without disassembly of the nanoparticle-peptide complex.