Undoped ZnO nanowire arrays and Al-doped ZnO nanostructures with nanowires and nanosheets were successfully synthesized on a polyethylene terephthalate substrate using the rapid hydrothermal synthesis. These undoped ZnO nanowire arrays showed close alignment with highly c-axis oriented and well-defined hexagonal facets (001). The coexistence of the nanowires and nanosheets was observed during the introduction of Al ions. The number of nanosheets increased due to the Al doping concentration and the lack of surface energy. The diameter of the nanosheets and the length of nanowire arrays also increased as a function of the growth time. Room-temperature photoluminescence spectra show that the ZnO:Al nanostructures on the ZnO seeded polyethylene terephthalate substrate yield low level of the defect density compared to the ZnO seeded glass substrate to remove post annealing process.