Zinc oxide (ZnO) has been widely investigated as an important ultraviolet (UV) sensing material in view of its wide band gap (~3.4 eV). However, the fabrication of continuous thin films of ZnO generally requires complex, time-consuming, and expensive processes, such as sputtering and atomic layer deposition. Herein, we demonstrate a bilayer film consisting of a conducting polymer and ZnO nanoparticles sequentially deposited using a simple, rapid, and inexpensive two-step spin-coating process. In this approach, it is not necessary to have a continuous ZnO nanoparticle film as the active layer, because the conducting polymer deposited under the ZnO nanoparticles acts as a conductive and continuous supporting layer for the particles. Poly(3,4-ethylenedioxythiophene) : polystyrene sulfonate (PEDOT: PSS) is used as the auxiliary layer to promote the efficient transport of photo-carriers generated from ZnO nanoparticles under UV light. As a result, under UV light (365 nm), photocurrents obtained from a ZnO/PEDOT: PSS bilayer film are significantly higher (~20 times) than that from a ZnO layer for a given voltage bias. The photoelectric performance can be further tuned by controlling the speed of spin-coating in the deposition of ZnO nanoparticles. The stability and photo response (rise and decay time) of the ZnO/PEDOT: PSS bilayer film under the repeated on-off condition are also reported.