Quantum dot nanoscale semiconductor heterostructures (QDHs) are a class of materials potentially useful for integration into solar energy conversion devices. However, realizing the potential of these heterostructured systems requires the ability to identify and synthesize heterostructures with suitably designed materials, controlled size and morphology of each component, and structural control over their shared interface. In this review, we will present the case for the utility and advantages of chemically synthesized QDHs for solar energy conversion, beginning with an overview of various methods of heterostructured material synthesis and a survey of heretofore reported materials systems. The fundamental charge transfer properties of the resulting materials combinations and their basic design principles will be outlined. Finally, we will discuss representative solar photovoltaic and photoelectrochemical devices employing QDHs (including quantum dot sensitized solar cells, or QDSSCs) and examine how QDH synthesis and design impacts their performance.