A growth scheme at a low processing temperature for high crystalline-quality of ZnO nanostructures can be a prime stepping stone for the future of various optoelectronic devices manufactured on transparent plastic substrates. In this study, ZnO nanorods (NRs) grown by the hydrothermal method at 150 °C through doping of transition metals (TMs), such as Co, Ni, or Co-plus-Ni, on polyethylene terephthalate substrates were investigated by various surface analysis methods. The TM dopants in ZnO NRs suppressed the density of various native defect-states as revealed by our photoluminescence and X-ray photoelectron spectroscopy analysis. Further investigation also showed the doping into ZnO NRs brought about a clear improvement in carrier mobility from 0.81 to 3.95 cm2/V-s as well as significant recovery in stoichiometric contents of oxygen. Ultra-violet photodetectors fabricated with Co-plus-Ni codoped NRs grown on an interdigitated electrode structure exhibited a high spectral response of ~137 A/W, on/off current ratio of ~135, and an improvement in transient response speed with rise-up and fall-down times of ~2.2 and ~3.1 s, respectively.