Photocatalysis technology is an effective method to remove pollutants in aquatic environment assisted by solar energy. Herein, the rhombohedral dodecahedral ZnO was dispersed on the g-C3N4 nanosheets for the construction of ZnO/g-C3N4 heterojunction via the combination of solvothermal method and calcination. The obtained ZnO/g-C3N4 heterojunction manifests excellent photocatalytic ability for methyl orange (MO). Especially, the optimal ZnO/g-C3N4 composite with the ZnO content of 10 wt% (ZC-3) exhibits the degradation efficiency of MO as high as 98.0% under visible-light of 60 min. A series of factors were all-around investigated, such as initial pH, photocatalyst dosage, initial MO concentration, organic anions, humic acid and other dyes. The photocatalytic degradation behavior of MO complies with the first-order reaction kinetics, and the apparent rate constant (kapp) of ZC-3 is 2.3 and 13.4 times than that of pure g-C3N4 and pure ZnO. Meanwhile, the ZnO/g-C3N4 heterojunction exhibits satisfactory cyclic stability and its photocatalytic mechanism is postulated. Therefore, the ZnO/g-C3N4 heterojunction possesses great economic utilization value and is expected to be widely used for wastewater remediation.