Synthesis of mesoporous anatase TiO2 beads via a simple two-step solution process without an additional calcination step is reported. The method involves a sol-gel and a hydrothermal techniques. Hexamine was used as the steric agent during the sol-gel process for the formation of the beads with controllable sizes. Also, the high water solubility of hexamine allows its easy removal, thus eliminating the existence of organic residue in the subsequent steps and the final product. The resulting beads were characterized using X-ray diffraction, high resolution scanning and transmission electron microscopy, X-ray absorption near edge structure analysis, and X-ray photoelectron spectroscopy. The beads were made into photoanodes with and without the addition of commercial TiO2 powders. We show an obvious efficiency enhancement in the resulting all-plastic flexible dye-sensitized solar cell, demonstrating that the obtained mesoporous anatase TiO2 beads with well-defined characteristics are an excellent candidate for energy applications. (C) 2014 The Electrochemical Society. All rights reserved.