In this work, anatase nanocrystallites are synthesized from an aqueous titanium(IV) chloride solution by hydrolysis and are used to fabricate mesoporous TiO2 film photoanodes. The aqueous-synthesized titania nanocrystallites possess high specific surface area (250-350 m(2)/g), 4-5 nm crystallite size, enlarged bandgap, and enhanced surface hydroxylation. Current-voltage measurements of dye-sensitized solar cells (DSSCs) based on the aqueous-synthesized titania showed higher photocurrent (13.0 mA/cm(2)) and conversion efficiency (5.0%) when compared to cells built from commercial Dyesol (10.7 mA/cm(2), 4.8%) or P25 (8.5 mA/cm(2), 4.1%) benchmark nanotitania materials. The enhanced performance is discussed in terms of improved dye loading and associated electron injection and transport facilitated by the nanocrystallite surface characteristics. (C) 2010 The Electrochemical Society. [DOI: 10.1149/1.3429249] All rights reserved.