- Hypothesis Subjecting colloids to electric fields often results in (electrophoretic) deposition on conductive substrates. Dispersing a single-source precursor (SSP) of choice in an appropriate solvent, should allow its deposition on different substrates. The SSP-solvent interaction might play a role in the deposition ( e.g. , direction, rate, coverage). After thermal decomposition, the SSPs convert to the designed material, thus allowing formation of thin films or hybrid nanostructures. Experiments Electrophoretic deposition (EPD) was applied on two representative SSPs in different solvents. These SSPs were deposited onto substrates covered with vertically-aligned ZnO nanorod (NR) arrays. After thermal decomposition, hybrid nanostructures were obtained and their morphology and interfaces were characterized by electron microscopy, X-ray diffraction, UV–vis, and electrochemistry. Findings Tuning the organic dispersant-SSP interaction allows control over the final film morphology, which can result in coating and filling of NRs with metal-sulfides or metal-oxides after thermal decomposition of the SSP. These findings introduce a new facile method for a fast and large-scale uniform deposition of different (nanostructured) thin film semiconductors on a variety of substrates. We discuss the influence of the dispersant medium on the deposition of metallo-organic SSPs. As an example, the formed ZnO–CdS interface supports charge transfer upon illumination.