A hydrothermal method was developed for the synthesis of bismuth titanate nanostructured microspheres. The precursor powder was prepared using a diethylene glycol mediated coprecipitation method. The as-synthesized nanostructured microspheres consisting of granular nanoparticles and nano-platelets were obtained through a hydrothermal treatment of the precursor powder in aqueous sodium hydroxide solution. Tailoring of the morphology was achieved by changing the precursor quantity, sodium hydroxide concentration, and reaction time. The formation mechanism of the nanostructured microspheres probably involves aggregation, followed by dissolution and recrystallization. X-ray diffraction, scanning electron microscopy and energy dispersive X-ray spectroscopy were used to characterize the phase purities, morphologies, and composition of the products.