ZnO nanomaterials are some of the most excellent candidates for low-cost but high-performance photodetectors, particularly in the UV region. Besides doping, architecting ZnO nanomaterials to extend their application is still attractive for developing low-cost optoelectronic devices. Thereby, this study introduces the innovation of ZnO nanorod-based photodetectors by combining two techniques, which are Cu doping and core/shell structuring. Particularly, the active material (ZnO/(Cu-doped ZnO) core/shell nanorods) was synthesized by a low-cost and easy fabrication process. Our device using the developed core/shell nanorods exhibits the maximum responsivity of ca. 4.5 mA W −1 at 395 nm light exposure, which is nearly 180% higher than that of a device based on Cu-doped ZnO NRs (formed with only the Cu-doping technique). This enhancement responsivity is attributed to the improved charge transport at the interface of the core/shell ZnO/(Cu-doped ZnO) NRs, which pertains to a process that reduces the electron−hole recombination probability, resulting in an improvement in the efficiency of the photodetectors. These outcomes reveal the essential role of core−shell structuring in improving the efficiency of ZnO-based photodetectors. In general, our study of ZnO/(Cu-doped ZnO) core/shell nanorods opens a potential approach for developing better photodetectors.