The structure and photocatalytic H-2 evolution property of a novel Zr-doped titanate nanobelt material fabricated by the dealloying method was studied. Using Ti-based metallic glassy powders as Ti and Zr source, the synthesized Na-2(Ti0.85Zr0.15)(4)O-9 and H-2(Ti0.85Zr0.15)(4)O-9 nanobelts show much higher photocatalytic activity than H2Ti4O9 nanobelts under UV irradiation. According to experimental results and first-principle calculations, the effect of Zr-doping on the band structure of these semiconductors was also investigated. The results show that Zr 4d orbitals played an effective role on both the valence and the conduction bands, which contributes to the enhanced photocatalytic activity. Furthermore, the H-2 evolution property is determined to be dominated by the synergetic influence of the thermodynamic driving force (band structure and H+ reduction potential) and the active reaction sites. Copyright (C) 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.