Electrospray pyrolysis, i.e. combination of electrospray and in-flight thermal treatment, has attracted much attention as a preparation method of functional ceramic particles. In this paper, we report the processing detail of spherical TiO2 nano- and microparticles by the electrospray pyrolysis method as well as their photocatalytic activity for hydrogen evolution. Titanium(IV) bis(ammonium lactato)dihydroxide aqueous solutions (TALH aq., 0.2-20 wt%) were injected into a capillary nozzle by a syringe pump (0.15-0.59 mL/min), and were electrosprayed by using DC 4 kV voltage, followed by the pyrolysis at 300-500 degrees C. Spherical TiO2 nano- and microparticles were successfully obtained. Effects of precursor-liquid concentration, liquid flow-rate, and pyrolysis temperature on the particle size, microstructure and functions were discussed. (C) 2011 Elsevier Ltd. All rights reserved.