We present the use of nanoparticle surface chemistry to mediate the deposition of metals onto colloidal nanoparticle substrates in patterns that are controlled by a supramolecular assembly on the colloid itself. These assemblies may be tuned either by ligand functionality or driven to phase transitions via electrochemical approaches. The solvent facing portion of these assemblies may also act as a selection agent in recruiting specific metals to the existing colloid surface. Combining these properties, we show several deposition motifs as well as broad metal generality using this surface chemistry based approach. We characterize this process and the resulting nanoparticle products using a combination of scanning probe microscopy, electorn microscopy, and nuclear magnetic resonance spectroscopy techniques. Applications in subsequent photomediated chemical processes will also be discussed.