in the materials science community. [2] Apart from the generation of H 2 and O 2 gases, photocatalysis can be extended to other applications. The early works on the irradiation of TiO 2 for purification of water via photocatalytic decomposition of pollutants were demonstrated by Frank and Bard in late 1970s. [3][4][5] These initial works and many reports later have shown that photooxidation of inorganic and organic contaminants is a promising route for environmental remediation. [6][7][8][9][10][11][12] In fact, the key factors that determine the efficiencies of a photocatalyst include its light harvesting capability and reduced charge carriers recombination of the photo generated electron-hole pairs. [3,13] However, TiO 2 possesses rather wide bandgap energies between 3.0 and 3.2 eV, with high photo activity only in the UV region (λ ≤ 390 nm) equivalent to only ≈5% of the solar spectrum. [14,15] Nevertheless, owing to its nontoxicity, low-cost synthesis, chemical inertness, and resistance against photocorrosion, TiO 2 has been long studied and recognized as the most promising photocatalyst material. [13,16] In order to harness more from the abundant renewable energy source, that is, solar energy, tremendous efforts have been devoted to reduce the bandgap energy of TiO 2 and broaden its optical absorption to the visible region. [8,[13][14][15]17,18] Bandgap engineering has been extensively carried out Ultrathin molybdenum oxyselenide (MoSe x O y ) coatings are made first ever by atomic layer deposition (ALD) within anodic 1D TiO 2 nanotube layers for photoelectrochemical and photocatalytic applications. The coating thickness is controlled through varying ALD cycles from 5 to 50 cycles (corresponding to ≈1-10 nm). In the ultraviolet region, the coatings have enhanced up to four times the incident photon-to-current conversion efficiency (IPCE), and the highest IPCE is recorded at 32% at (at λ = 365 nm). The coatings notably extend the photoresponse to the visible spectral region and remarkable improvement of photocurrent densities up to ≈40 times is registered at λ = 470 nm. As a result, the MoSe x O y -coated-TiO 2 nanotube layers have shown to be an effective photocatalyst for methylene blue degradation, and the optimal performance is credited to a coating thickness between 2 and 5 nm (feasible only by ALD). The enhancement in photoactivities of the presented heterojunction is mainly associated with the passivation effect of MoSe x O y on the TiO 2 nanotube walls and the suitability of bandgap position between MoSe x O y and TiO 2 interface for an efficient charge transfer. In addition, MoSe x O y possesses a narrow bandgap, which favors the photoactivity in the visible spectral region.