Two kinds of CNT/TiO2 composite photocatalysts were synthesized with multi-walled carbon nanotubes (MWCNTs) and titanium(IV) n-butoxide (TNB) by a MCPBA oxidation method. Since MWCNTs had charge transfer and semiconducting, the CNT/TiO2 composite shows a good photo-degradation activity. The XRD patterns reveal that only anatase phase can be identified for MCT composite, but the HMCT composite synthesized with HCl treatment was observed the mixed phase of anatase and rutile. The EDX spectra were shown the presence as major elements of Ti with strong peaks. From the SEM results, the sample MCT and HMCT synthesized by the thermal decomposition with TNB show a homogenous sample with only individual MWCNTs covered with TiO2 without any jam-like aggregates between CNTs and TiO2. From the photocatalytic results, we could be suggested that the excellent activity of the CNT/TiO2 composites for organic dye and UV irradiation time could be attributed to combination effects between TiO2 and MWCNTs with plausible photodegradation mechanism.