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Aligned TiO 2  nanotube layers (TiNTs) grown by self‐organizing anodization of a Ti‐substrate in a fluoride‐based electrolyte were decorated with graphitic‐phase C 3 N 4  (g‐C 3 N 4 ) via a facile chemical vapor deposition approach. In comparison with classical TiO 2  nanotubes (anatase), the g‐C 3 N 4 /TiNTs show an onset of the photocurrent at 2.4 eV (vs. 3.2 eV for anatase) with a considerably high photocurrent magnitude in the visible range. After further decoration with Pt nanoparticles, we obtained a visible‐light responsive platform that showed, compared with g‐C 3 N 4 ‐free TiNTs, a strong enhancement for photoelectrochemical and bias‐free H 2  evolution (15.62 μLh −1  cm −2 ), which was almost a 98‐fold increase in the H 2  production rate of TiNTs (0.16 μLh −1  cm −2 ). In a wider context, the g‐C 3 N 4 ‐combined 3 D nanoporous/nanotubular structure thus provides a platform with significant visible‐light response in photocatalytic applications.

Pt‐Decorated g‐C 3 N 4 /TiO 2 Nanotube Arrays with Enhanced Visible‐Light Photocatalytic Activity for H 2 Evolution