Nano-architectures of single-crystalline anatase TiO2 nanosheets predominantly exposing the {001} facet are constructed in well-oriented configurations based on the strategies of controlled growth of TiO2 in novel growth modes, i.e. (a) the epitaxial growth mode of TiO2 nanosheets on the surface of oriented crystalline substrates, TiO2 and SnO2, resulting in an ordered growth direction, and (b) the hierarchical growth mode of TiO2 nanosheets on oriented nano-crystals, TiO2 nanowires, resulting in a well-ordered orientation and high surface areas as compared with conventional random growth of nanosheets. The present work explores a variety of methods for morphology control of TiO2 nanosheets directly grown on nanostructures as mother components, on which the potential of anatase TiO2 nanosheets to expose a high fraction of the reactive {001} facet is maximized.