TiO nanoribbons (TiO NRs) loaded with FeCo-AlO catalyst were synthesized and used as a precursor in the synthesis of TiO nanoribbons/carbon nanotubes (TiO NRs/CNTs) composite by a chemical vapor deposition (CVD) method. TiO NRs and TiO NRs/CNTs composite were characterized by XRD, FT-IR, TEM, SEM, EDX and UV-Vis spectrophotometer. The results revealed the formation of TiO-B and hydrogen titanate nanoribbon like structures by the hydrothermal treatment. After loading TiO NRs by FeCo-AlO catalyst and the CVD growth of carbon nanotubes, the synthetic TiO nanoribbons converted entirely to TiO-B nanoribbons with nanopits structure. The composite composed of tube-like nanostructures forming an interlocked network from CNTs and TiO-B NRs. The composite shows a relatively red-shifted band gap (3.09 eV), broader and stronger UV absorption band relative to TiO NRs. The photocatalytic properties of TiO NRs and TiO NRs/CNTs composite were studied under sunlight irradiation. The photocatalytic degradation of methylene blue (MB) dye was investigated as a function of contact time, dye concentration, and catalyst dose. The kinetics and mechanisms of degradation were discussed. TiO NRs/CNTs composite showed higher stability after six runs and 50% shorter irradiation time than TiO NRs photocatalyst.