ZnO decorated-TiO2 nanosheets with exposed {001} facets were achieved by a simple hydrothermal method. The size and shape of ZnO nanoparticles were controlled by tuning the growth temperature. SEM, HRTEM, and SAED measurements confirmed the formation of {001} TiO2 nanosheets with the decoration of ZnO nanoparticles. The ZnO/TiO2 {001} facets heterostructures show an improved efficient in photocatalytic activities due to the decreased charge recombination with the presence of ZnO nanocrystals.