Previous research has shown that the hybridization of N 2p and O 2p orbitals effectively suppresses the electrical activity of oxygen vacancies in oxide semiconductors. However, achieving N-alloyed Ga2O3 films, known as GaON, poses a significant challenge due to nitrogen's limited solubility in the material. In this study, a new method utilizing plasma-enhanced chemical vapor deposition with high-energy nitrogen plasma was explored to enhance the nitrogen solubility in the material. By adjusting the N2 and O2 carrier gas ratio, we could tune the thin film's bandgap from 4.64 to 3.25 eV, leading to a reduction in the oxygen vacancy density from 32.89% to 19.87%. GaON-based photodetectors exhibited superior performance compared to that of Ga2O3-based devices, with a lower dark current and a faster photoresponse speed. This investigation presents an innovative approach to achieving high-performance devices based on Ga2O3.