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CuAlO₂ was synthesized by a hydrothermal method, in which the Cu–O dimers were incorporated by simply altering the ratio of the reactants and the temperature. The incorporation process increases the grain size in CuAlO₂, and modulates the work function and binding energies for CuAlO₂ due to the partial substitution of Cu⁺ 3d¹⁰ with Cu²⁺ 3d⁹ orbitals in the valence band maximum by alloying non-isovalent Cu–O with a CuAlO₂ host. Based on the ZnO nanorod arrays (NRs) ultraviolet photodetector, CuAlO₂/Cu–O fabricated by the low-cost drop-coating method was used as the p-type hole transport layer. The incorporation of the Cu–O clusters into CuAlO₂ lattice to enhance the conductivity of CuAlO₂ is an effective way for improving ZnO NRs/CuAlO₂ device performance. The photodetectors exhibit significant diode behavior, with a rectification ratio approaching 30 at ±1 V, and a dark saturation current density 0.81 mA cm⁻². The responsivity of the ZnO-NRs-based UV photodetector increases from 13.2 to 91.3 mA/W at 0 V bias, with an increase in the detectivity from 2.35 × 10¹⁰ to 1.71 × 10¹¹ Jones. Furthermore, the ZnO NRs/[CuAlO₂/Cu–O] photodetector exhibits a maximum responsivity of 5002 mA/W at 1.5 V bias under 375 nm UV illumination.