Dispersion of exfoliated CN over the surface of exfoliated LDH composite materials, and its photocatalytic water splitting under visible-light irradiation. Exploiting the advantage of a layered architecture, layered graphitic carbon nitride (CN) and NiFe-layered double hydroxide (LDH) have been coupled in the present investigation to design a series of highly efficient novel CNLDH composites for visible light-induced photocatalytic H 2 and O 2 evolution. The syntheses of these composites were carried out using a facile weight impregnation method while varying the wt% of CN on LDH. The structural, optical, and morphological properties of these composites were characterized by various physicochemical techniques. The results indicate a tuned-in band gap energy within the range of pure LDH to pure CN. In addition, the remarkable quenching of the PL signal and prolonged photogenerated charge lifetime confirmed by TRPL spectra demonstrates the excellent photocatalytic activity of these composites. The activity could be ascribed to the dispersion of exfoliated CN over the brucite layer of LDH, in which strong energy transfer takes place in terms of charge carriers. The visible light-induced photocatalytic H 2 and O 2 evolution study resulted in an enhancement in the activity of the CNLDH10 composite with a H 2 evolution rate of 1488 μmol 2 h −1 and O 2 evolution rate of 886 μmol 2 h −1 . The high photocatalytic activities of these composites may be due to good dispersion of exfoliated CN over the brucite layer of edge-shared MO 6 octahedra, higher life time of charge carriers, low PL intensity, appropriate band gap energy and enhancement in photocurrent density.