Solar energy-driven practices using semiconducting materials is an ideal approach toward wastewater remediation. In order to attain a superior photocatalyst, a composite of g-C 3 N 4 and ZnO (GCN−ZnO) has been prepared by one-step thermal polymerization of urea and zinc carbonate basic dihydrate [ZnNO 3 ] 2 •[Zn(OH) 2 ] 3 . The GCN−ZnO0.4 sample showed an evolved morphology, increased surface area (116 m 2 g −1 ), better visible light absorption ability, and reduced band gap in comparison to GCN−pure. The GCN−ZnO0.4 sample also showed enhanced adsorption and photocatalytic activity performance, resulting in an increased reaction rate value up to 3 times that of GCN−pure, which was attributed to the phenomenon of better separation of photogenerated charge carriers resulting because of heterojunction development among interfaces of GCN−pure and ZnO. In addition, the GCN−ZnO0.4 sample showed a decent stability for four cyclic runs and established its potential use for abatement of organic wastewater pollutants in comparison to GCN− pure.