This work focuses on increasing the quantum efficiency in titania photosynthetic (photosplitting of water) and photocatalysts for photocatalytic (oxidation of acetaldehyde) reactions by synthesizing controlled anatase nanocrystals with a shoebox-like shape. In general, anatase crystals have tetragonal dipyramid shapes (see figure). All of the {101} surfaces have the same property, because they are symmetrically identical. The elongated anatase crystals are synthesized through topological replacement (or transformation) of titanate display shoebox-like shapes with crystal forms of {100} and {001} (see figure). The {001} and {100} surfaces have different physical/chemical properties because they are not symmetrically related. The difference will enhance the electron-hole separation generated by photons and therefore enhance the quantum efficiency of photocatalytic reactions. In addition, both {001} and {100} surfaces have higher energies than normal {101} surfaces, which increases surface reactivity of the anatase. The shape-controlled anatase crystals display enhanced reactivity for both photosplitting of water and photocatalytic oxidation of organic pollutants (such as volatile organic compounds in air) using renewable solar energy. The results have important implications for enhancing the photocatalytic activity of titania for environmental remediation, increasing the quantum efficiency in photovoltaic solar cells and other photoassisted processes.