The formation mechanism and photocatalytic properties of a multiwalled carbon nanotube (MWCNT)/TiO2- based nanotube (TNTs) composite are investigated. The CNT/TNT composite is synthesized via a solution chemical route. It is confirmed that this 1-D nanotube composite has a core-shell nanotubular structure, where the TNT surrounds the CNT core. The photocatalytic activity investigated based on the methylene blue degradation test is superior to that of with pure TNT. The CNTs play two important roles in enhancing the photocatalytic activity. One is to act as a template to form the core-shell structure while titanate nanosheets are converted into nanotubes. The other is to act as an electron reservoir that facilitates charge separation and electron transfer from the TNT, thus decreasing the electronhole recombination efficiency.