Oppositely charged 2D inorganic nanosheets of ZnAl-layered double hydroxide and layered titanate were successfully assembled into an interstratified nanohybrid through simply mixing the corresponding nanosheet suspensions. Powder X-ray diffraction and high-resolution transmission electron microscope clearly revealed that the component nanosheets in the as-obtained nanohybrid ZnAl-Ti3O7 retain the 2D sheet skeletons of the pristine materials and that the two kinds of nanosheets are well arranged in a layer-by-layer alternating fashion with a basal spacing of about 1.3 nm, coincident with the thickness summation of the two component nanosheets. The effective interfacial heterojunction between them and the high specific surface area resulted in that the nanohybrid exhibits a superior photocatalytic activity in the degradation of methylene blue with a reaction constant k of 2.81 x 10(-2) min(-1), which is about 9 and 4 times higher than its precursors H2Ti3O7 and ZnAl-LDH, respectively. Based on UV-vis, XPS and photoelectrochemical measurements, a proposed photoexcitation model was provided to understand its photocatalytic behavior. (C) 2014 Elsevier B.V. All rights reserved.