The principal impetus for the fabrication of functional nanotube materials comes from the promise of discovering unique structure-dependant properties and superior performance that are derived from their intrinsic nanotubular architecture. [1][2][3][4] 1D TiO 2 nanotube arrays prepared by the electrochemical anodization of self-organized porous structures on Ti foil [5][6][7] have attracted great research interest in recent years owing to their peculiar architecture, remarkable properties, and potential for wide-ranging applications. Uniform TiO 2 nanotubes are quite remarkably different in structure from other forms of TiO 2 , and are highly ordered, high-aspect-ratio structures with nanocrystalline walls perpendicular to electrically conductive Ti substrates, thereby naturally forming a Schottky-type contact. Moreover, these structures can be directly used as electrodes for photoelectric applications since the size of the nanotubes is very precisely controllable. The technological applications of TiO 2 nanotube arrays are still at an early stage, but these remarkable structures have already been shown to be very promising for applications in sensing, [8] catalysis, [9] photovoltaics, [10] photoelectrolysis, [11] and nanotemplating. [12] The electrical resistance of the TiO 2 nanotubes changes by almost 7 orders of magnitude upon exposure to 1000 ppm H 2 , [13] the largest ever reported sensitivity of a material to a gas. Furthermore, the H 2 evolution rate of TiO 2 nanotube arrays has been reported to be 76 mL hw -1 , [11] which is the highest reported H 2 generation rate for any oxide system upon photoelectrolysis. TiO 2 nanotube arrays have also attracted great interest for enhancing the photocatalytic degradation of various organics, which makes them promising materials for the detection of pollutants. Given the increasing quantities of pollutants that are being dumped into water bodies, environmental monitoring and control have become issues of global concern. Chemical oxygen demand (COD) is one of the most widely used metrics in the field of water-quality analysis in many countries, and is frequently used as an important index for controlling the operation of wastewater treatment plants, wastewater effluent monitoring, and taxation of wastewater pollution. [14] or ultrasound-assisted oxidation.[15]Other alternative assays have also been developed such as electrocatalytic determination using PbO 2 or Cu sensors in thin-cell reactors, [16,17] and photocatalytic and photoelectrocatalytic methods based on TiO 2 nanomaterial sensors. [18,19] However, all these modified K 2 Cr 2 O 7 methods are still plagued by the secondary pollution caused by highly toxic Cr(VI) ions, and moreover, the PbO 2 sensors pose the risk of the potential release of hazardous Pb during the preparation and disposal of the active material of the sensors. As compared to traditional analytical methods, photoelectrocatalytic approaches are more promising because of the superior oxidative abilities of illuminated TiO 2 . Furthermore, TiO 2 ...