In this work, we successfully synthesized a novel ZnCr-LDH/N-doped graphitic carbon-incorporated g-C3N4 (g-C3N4-C(N)) hybrid with unique two-dimensional/two-dimensional (2D-2D) structure for the efficient degradation of Congo red under visible light irradiation. It was demonstrated that ZnCr-LDH/g-C3N4-C(N) exhibited lower photogenerated electron-hole recombination rate and enhanced light harvesting. Furthermore, its derived calcined product also showed outstanding performance due to the unique heterogeneous structure and the synergistic effect between photocatalysis and adsorption. In addition, the mixed metal oxide ZnO and ZnCr2O4 in ZnCr-CLDH/g-C3N4-C(N) dispersed uniformly on the g-C3N4-C(N) exposed more active sites and facilitated the photodegradation of pollutants.