Multi-walled carbon nanotubes-titanium dioxide (MWCNTs-TiO2) nanocomposites were synthesized via microwave-assisted synthesis and conventional hydrothermal method, comprising of well-crystallized anatase TiO2 nanoparticles with different MWCNTs contents. TiO2 nanoparticles synthesized by the rapid thermal decomposition of tetra-butyl titanium (Ti(OC4H9)4) in the presence of acid treated MWCNTs, were attached on the surface of MWCNTs by means of chemical bonds under microwave irradiation. The addition of MWCNTs did not influence the structure of anatase TiO2. The photocatalytic performance evaluation of composite materials was conducted under UV and visible light using methyl orange (MO) as a typical pollutant. The enhancement in photocatalytic efficiency of nanocomposites was clearly observed by the presence of MWCNTs, which could contribute to improve the adsorption of MO dye, absorption of more light and also obstruct the photogenerated electron-hole pair's recombination.