This paper provides a continuous method for grafting carbon nanotubes (CNTs) on the surface of carbon fibers by chemical vapor deposition (CVD). The control of the morphology of CNTs/CFs can be achieved by adding thiourea to the cobalt nitrate precursor. The sulfur can increase the catalytic activity of the Co catalyst. Scanning electron microscopy reveals that a uniform layer of CNTs is grafted onto the surface of carbon fibers with the presence of thiourea. Through the single-filament tensile strength test, it can be found that the tensile strength of the fiber is increased by up to about 10% compared with the desized carbon fibers after the CVD process. And the reason for the enhancement is explored through X-ray diffraction. Raman spectroscopy reveals that the sample possesses the highest degree of graphitization at a thiourea concentration of 0.02 mol/L. It is found by high-resolution transmission electron microscopy that the growth mechanism of CNTs is tip growth mechanism, and the diameter of the CNTs is about 15 nm.