The present work reports nitrogen doping of self-organized TiO2 nanotubular layers. Different thicknesses of the nanotubular layer architecture were formed by electrochemical anodization of Ti in different fluoride-containing electrolytes; tube lengths were 500 nm, 2.5 μm, and 6.1 μm. As-formed nanotube layers were annealed to an anatase structure and treated in ammonia environment at 550 °C to achieve nitrogen doping. The crystal structure, morphology, composition and photoresponse of the N-doped were characterized by scanning electron microscopy, x-ray diffraction, x-ray photoelectron spectroscopy, and photoelectrochemical measurements. Results clearly show that successful N-doping of the TiO2 nanotubular layers can be achieved upon ammonia treatment. The magnitude of the photoresponse in ultraviolet and visible light is strongly dependent on the thicknesses of the layers. This effect is ascribed to recombination effects along the tube length.