The organic capping ligand and nanomorphology of semiconductor nanocrystals play a key role in dictating interfacial charge transfer processes in hybrid semiconductor nanocrystal/polymer-based photovoltaic devices. This Perspective discusses recent results related to advances in quantized semiconductor nanocrystal/polymer solar cells and their efficiency. Moreover, characterization of the interfacial charge transfer processes that limit device efficiency and their relationship to film nanomorphology is also discussed.