Although ZnO and ZnS are abundant, stable, environmentally benign, their band gap energies (3.44 eV, 3.72 eV) are too large for optimal photovoltaic efficiency. By using band-corrected pseudopotential density-functional theory calculations, we study how the band gap, optical absorption, and carrier localization can be controlled by forming quantum-well like and nanowire-based heterostructures of ZnO/ZnS and ZnO/ZnTe. In the case of ZnO/ZnS core/shell nanowires, which can be synthesized using existing methods, we obtain a band gap of 2.07 eV, which corresponds to a Shockley-Quiesser efficiency limit of 23%. Based on these nanowire results, we propose that ZnO/ZnS core/shell nanowires can be used as photovoltaic devices with organic polymer semiconductors as p-channel contacts.