In this study we report the synthesis of a series of composite nanostructures comprising LDH and TiO2 phases. The materials characterization showed that the LDH crystallites are encapsulated inside the TiO2 matrix after the anatase seeds are deposited on MgxAl-LDHs. The structure in which LDH phase is embedded into anatase matrix is unique bringing important advantages to the photocatalytic performances of the nanocomposites. The photocatalytic activity of the prepared nanocomposites was tested on the degradation of the methylene blue (MB) in aqueous solution. The photocatalytic activities of the nanocomposites were compared with commercial TiO2 nanoparticles Degussa P25. The nanocomposites exhibited superior photocatalytic activity in basic environment because the negatively charged surface of TiO2 nanoparticles at high pH attracts the positively charged methylene blue species.