Highly efficient photocatalysts for visible light-induced O2 generation are synthesized via an electrostatically derived self-assembly of Zn–Cr-LDH 2D nanoplates with graphene 2D nanosheets. In the obtained nanohybrids, the positively charged Zn–Cr-LDH nanoplates are immobilized on the surface of negatively charged graphene nanosheets with the formation of a highly porous stacked structure. A strong electronic coupling of the subnanometer-thick Zn–Cr-LDH nanoplates with reduced graphene oxide (RGO)/graphene oxide (GO) nanosheets gives rise not only to the prominent increase of visible light absorption but also to a remarkable depression of the photoluminescence signal. The self-assembled Zn–Cr-LDH–RGO nanohybrids display an unusually high photocatalytic activity for visible light-induced O2 generation with a rate of ∼1.20 mmol h−1 g−1, which is far superior to that of the pristine Zn–Cr-LDH material (∼0.67 mmol h−1 g−1). The fact that pristine Zn–Cr-LDH is one of the most effective visible light photocatalysts for O2 production with unusually high quantum efficiency of 61% at λ = 410 nm highlights the excellent functionality of the Zn–Cr-LDH–RGO nanohybrids as visible light active photocatalysts. The Zn–Cr-LDH–RGO nanohybrid shows a higher photocatalytic activity than the Zn–Cr-LDH–GO nanohybrid, providing strong evidence for the superior advantage of the hybridization with RGO. The present findings clearly demonstrate that graphene nanosheets can be used as an effective platform for improving the photocatalytic activity of 2D nanostructured inorganic solids.