Epitaxially-oriented CdSe quantum dots (ca. 5 nm diameter) with controllable spatial distribution and narrow size distribution have been electrodeposited on evaporated gold substrates. The degree of aggregation of the nanocrystals can be controlled by the deposition temperature and current density. All the nanocrystals deposited on a single gold crystallite are of the wurtzite structure with the basal plane parallel to the gold {111} plane and with the same azimuthal orientation. This simple and convenient method of preparing oriented quantum dots provides an effective means for studying the transition between molecular and bulk properties, as well as a new surface architecture on the nanometer scale.