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. (C) 2018 Elsevier Inc. All rights reserved.