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 mmol 2 h À1 and O 2 evolution rate of 886 mmol 2 h À1 . 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. of electrons and holes. 5 The common layered structures of ZnCr-LDH and layered titanate enable an effective physical contact and a strong electronic coupling between them, which is effective in enhancing the photocatalytic activity of ZnCr-LDH. This motivated us to take the challenge of designing composite photocatalysts by coupling LDH with other layered semiconductor materials, like metal-free polymeric graphitic carbon nitride (g-C 3 N 4 ), which has an appropriate band gap of 2.7 eV and optical absorption in the visible region. 18 The g-C 3 N 4 material also possesses very high thermal, mechanical and chemical stability. Many studies have been focused on the applications of g-C 3 N 4 materials in photocatalytic water splitting together with degradation of organic pollutants. [19][20][21][22] However, recent studies have indicated that these materials exhibit photocatalytic activities for both H 2 and O 2 evolution under visible light irradiation in the presence of a sacricial donor and acceptor. 23 Several composite materials coupled with g-C 3 N 4 have also been reported, such as g-