Colloidal quantum dots (CQDs) offer a path toward high-efficiency photovoltaics based on low-cost materials and processes. Spectral tunability via the quantum size effect facilitates absorption of specific wavelengths from across the sun's broad spectrum. CQD materials' ease of processing derives from their synthesis, storage, and processing in solution. Rapid advances have brought colloidal quantum dot photovoltaic solar power conversion efficiencies of 6% in the latest reports. These achievements represent important first steps toward commercially compelling performance. Here we review advances in device architecture and materials science. We diagnose the principal phenomenon-electronic states within the CQD film band gap that limit both current and voltage in devices-that must be cured for CQD PV devices to fulfill their promise. We close with a prescription, expressed as bounds on the density and energy of electronic states within the CQD film band gap, that should allow device efficiencies to rise to those required for the future of the solar energy field. © 2011 American Chemical Society.