ZnCr layered double hydroxides (ZnCr LDH) nanosheets modified graphitic carbon nitride (g-C3N4) nanohybrids were fabricated via a self-assembly procedure through electrostatic interaction between these two components. Such 2D-2D inorganic-organic hybrid material was employed for photocatalytic hydrogen production under visible light for the first time. The physical and photophysical properties of the hybrid nanocomposites were investigated to reveal the effect of ZnCr LDH nanosheets on the photocatalytic activities of g-C3N4. It was found that 1 wt% ZnCr LDH nanosheets modified g-C3N4 was optimal for the formation of intimate interfacial contact. The visible light photocatalytic H-2 production activity over g-C3N4 was enhanced about 2.8 times after ZnCr LDH nanosheets modification. The significant enhancement in photocatalytic performance for ZnCr LDH/g-C3N4 hetero-junction should be attributed to the promoted charge transfer and separation efficiency, resulting from the intimate interfacial contact and Type II band alignment between ZnCr LDH and g-C3N4. (C) 2017 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.