Environmental pollution, especially water pollution, is becoming increasingly serious. Organic dyes are one type of the harmful pollutants that pollute groundwater and destroy ecosystems. In this work, a series of graphitic carbon nitride (g-C3N4)/ZnO photocatalysts were facilely synthesized through a grinding method using ZnO nanoparticles and g-C3N4 as the starting materials. According to the results, the photocatalytic performance of 10 wt.% CN-200/Z-500 (CN-200, which g-C3N4 was 200 kGy, referred to the irradiation metering. Z-500, which ZnO was 500 °C, referred to the calcination temperature) with the CN-200 exposed to electron beam radiation was better than those of either Z-500 or CN-200 alone. This material displayed a 98.9% degradation rate of MB (20 mg/L) in 120 min. The improvement of the photocatalytic performance of the 10 wt.% CN-200/Z-500 composite material was caused by the improvement of the separation efficiency of photoinduced electron–hole pairs, which was, in turn, due to the formation of heterojunctions between CN-200 and Z-500 interfaces. Thus, this study proposes the application of electron-beam irradiation technology for the modification of photocatalytic materials and the improvement of photocatalytic performance.