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Regularly spaced TiO 2  nanotubes were prepared by anodizing a titanium substrate in triethylene glycol electrolyte at elevated temperature. In comparison to conventional TiO 2  nanotubes, spaced nanotubes possess an adjustable spacing between the individual nanotubes; this allows for controlled buildup of a hierarchical nanoparticle‐on‐nanotube structure. Here, we use this principle for layer‐by‐layer decoration of the tubes with TiO 2  nanoparticles. The hierarchical structure after N doping and NH 3  treatment at 450 °C shows a significant enhancement of visible‐light absorption, although it only carries a low doping concentration of nitrogen. For optimized N‐doped and particle‐decorated spaced TiO 2  nanotubes, a considerable improvement in photocatalytic activity is obtained in comparison with conventional N‐doped TiO 2  nanotubes or comparable N‐doped nanoparticle films. This is attributed to an enhanced visible‐light absorption through the N‐doped nanoparticle shell and a fast charge separation between the shell and the one‐dimensional nanotubular core.

Spaced Titania Nanotube Arrays Allow the Construction of an Efficient N‐Doped Hierarchical Structure for Visible‐Light Harvesting