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We present a novel method for synthesizing epitaxial quantum dot-nanowire (QD-NW) heterostructures using the example of colloidal PbSe QDs decorated on furnace-grown hematite (α-Fe2O3) NWs. The direct heterogeneous nucleation of QDs on Fe2O3 NWs relies upon an aggressive surface dehydration of the as-synthesized Fe2O3 NWs at 350 °C under vacuum and subsequent introduction of colloidal reactants resulting in direct growth of PbSe QDs on Fe2O3. The synthesis is tunable: the QD diameter distribution and density of QDs on the NWs increase with increased dehydration time, and QD diameters and size distributions decrease with decreased injection temperature of the colloidal synthesis. Transmission electron microscopy (TEM) structural analysis reveals direct heteroepitaxial heterojunctions where the matching faces can be PbSe (002) and Fe2O3 (003) with their respective [11̅0] crystallographic directions aligned. This can be a general approach for integrating colloidal and furnace synthetic techniques, thus broadening possible material combinations for future high-quality, epitaxial nanoscale heterostructures for solar applications.