Electron transfer at the interface between a photoactive molecule and large bandgap nanostructured metal oxide semiconductors (ZnO, TiO2 for instance) remains at the center of intense research in numerous areas of solar energy conversion. Such areas encompass photocatalysis and solar fuels, photovoltaics, energy storage, and artificial photosynthesis. An enduring challenge is the ability to achieve control of the chromophore/semiconductor interface at the molecular level. The goal of our collaborative research is to address it by a combination of synthetic design and interfacial charge transfer studies. The presentation will describe the development of “functional” linkers for chromophore-linker model compounds that are able to tune and control the energy level alignment of molecules on nanostructured or single crystal inorganic semiconductors.