Zinc oxide (ZnO) is a material of great interest for short-wavelength optoelectronic applications due to its wide band gap (3.37 eV) and high exciton binding energy (60 meV). Due to the difficulty in stable p-type doping of ZnO, other p-type materials such as gallium nitride (GaN) have been used to form heterojunctions with ZnO. p-GaN/n-ZnO heterojunction devices, in particular light-emitting diodes (LED) have been extensively studied. There was a huge variety of electronic properties and emission colors on the reported devices. It is due to the different energy alignment at the interface caused by different properties of the GaN layer and ZnO counterpart in the junction. Attempts have been made on modifying the heterojunction by various methods, such as introducing a dielectric interlayer and post-growth surface treatment, and changing the growth methods of ZnO. In this study, heterojunction LED devices with p-GaN and ZnO nanorods array are demonstrated. The ZnO nanorods were grown by a solution method. The ZnO nanorods were exposed to different kinds of plasma treatments (such as nitrogen and oxygen) after the growth. It was found that the treatment could cause significant change on the optical properties of the ZnO nanorods, as well as the electronic properties and light emissions of the resultant LED devices.