CdSe/CdS core/shell quantum dots have been synthesized and assembled onto pre-functionalized gold surfaces by either hydrogen bonding or covalent bonds through different functional groups. Control of the conditions during the deposition process allows producing a high coverage of quantum dots via molecular linkages. The quantum-dot surface is highly photoactive and is used in a surface sensitized Schottky barrier photovoltaic structure as the photoreception component. Atomic force microscopy (AFM) and X-ray photoelectron Spectroscopy (XPS) are used to characterize and confirm the morphology and linkage of the assemblies on Au surfaces. The electron transfer from the quantum-dot layer to the Schottky barrier device is examined by measuring the current-voltage (IV) curve of such photovoltaic devices under simulated sun light.