Scintillators, which convert high-energy rays such as X-rays and positrons into visible and ultraviolet light, are incorporated as radiation detectors in X-ray computer tomography (X-ray CT) and positron emission tomography (PET), in which system performance highly depends on the characteristics of the scintillator used. In this study, SrGa2S4:Eu/ZnO vertical nanowire (ZnO-vnw) bilayer scintillators were fabricated by electrodeposition of ZnO-vnw followed by electrophoresis deposition of SrGa2S4:Eu particles, and their structure, optical properties, and scintillator characteristics were evaluated. The ZnO-vnw were composed of vertically aligned ZnO nanowires with an excellent (001) out-of-plane orientation, and the SrGa2S4:Eu layer was composed of particles adhered to the ZnO-vnw. The SrGa2S4:Eu/ZnO-vnw bilayer scintillators emitted visible light at a wavelength of 533 nm with a lifetime of 0.389 s and functioned as a scintillator for X-ray irradiation. The resolution and luminescence intensity of the SrGa2S4:Eu/ZnO-vnw bilayer scintillators were improved by the introduction of the ZnO-vnw layer, when compared with those of the ZnO-vnw-free-SrGa2S4:Eu layer, when the thickness ratio of SrGa2S4:Eu layer to ZnO-nw length were 1.1~1.3. The SrGa2S4:Eu/ZnO-vnw bilayer scintillator revealed a spatial resolution of 6.8 μm, which was slightly larger than 5.4 μm of a ready-made LuAG single-crystal scintillator.