This study presents the positive effects of proton/electron irradiation on the crystallinity of GaP-based dilute nitride alloys. It is found that proton/electron irradiation followed by rapid thermal annealing enhances the PL peak intensity of GaPN alloys, whereas major photovoltaic III-V materials such as GaAs and InGaP degrade their crystal quality by irradiation damage. Atomic force microscopy and transmission electron microscopy reveal no degradation of structural defects. GaAsPN solar cell test devices are then fabricated. Results show that the conversion efficiency increases by proton/electron irradiation, which is mainly caused by an increase in the short-circuit current.