Ni-doped and Ni/Cr co-doped TiO2 nanotubes were successfully synthesized using a novel hydrothermal method. The surface and bulk properties of as-synthesized nanopowders were characterized using various microstructural and optical techniques. The photocatalytic ability of these nanopowders was investigated systematically for the decomposition of methylene blue dye (MB) under visible light illumination. The morphological results revealed the structural transformation of TiO2 nanotubes to nanosheets, and further to a mixture of nanosheet/nanotube on doping with Ni and co-doping of Ni/Cr, respectively. Moreover, the Ni doping causes an optical absorption edge shifts towards lower wavelengths, while doping by Ni/Cr results to an optical absorption edge shifts towards higher wavelength in comparison to TiO2-nanotubes. Also, Ni-doping and Ni/Cr co-doping strongly affects the Raman vibrational modes owing to the changes in interplanar distance, crystallite size, dislocation density, and crystal microstrains. Among the undoped, doped and co-doped TiO2 nanoparticles, the 6Ni/4Cr co-doped TiO2 exhibited a higher efficiency of 95.6% and excellent stability towards the photocatalytic degradation of MB. It is attributed to the availability of many carriers for the efficient photo-oxidation within the UV-Vis optical absorption range. Also, the photocatalytic reaction kinetics and degradation mechanism of MB were discussed. (C) 2019 Elsevier Inc. All rights reserved.