Methanol oxidation performance of a carbon-supported Pt-Ru alloy catalyst used at the direct methanol fuel cell (DMFC) anode is improved by adding TiO2. However, the methanol oxidation performance of the electrocatalyst described above must be enhanced further to realize practical application in DMFCs. In this study, we used our original surface-modifying technique termed the "polygonal barrel-sputtering method" to prepare a carbon-supported Pt-Ru and TiO2 (Pt-Ru/TiO2/C) electrocatalyst offering higher methanol oxidation performance. The obtained results show that the methanol oxidation performance of the prepared Pt-Ru/TiO2/C is superior to that using wet process as the TiO2 deposition method. Furthermore, for our sputtering method, the peak current of methanol oxidation on the Pt-Ru/TiO2/C is enhanced by increasing the TiO2 deposited amount up to 2.8 wt.%. These results suggest that a Pt-Ru/TiO2 interface area is increased using the polygonal barrel-sputtering method, providing the high methanol oxidation performance of Pt-Ru/TiO2/C. (C) 2010 Elsevier Ltd. All rights reserved.