A large-scale carbon nanotube/CoFe2O4 (CNTs/CoFe2O4) spinel nanocomposite has been fabricated by a chemical vapor deposition method using CoFe2O4 nanoparticles as catalysts. A uniform mixture of CNTs and CoFe2O4 nanoparticles was obtained simultaneously. The structure and chemical composition of the product were investigated using various techniques, such as x-ray diffraction, high-resolution transmission electron microscopy, and electron energy loss spectroscopy. It was found that the particles functionalized on CNTs were cubic phase CoFe2O4. Microwave absorption of the CNT/CoFe2O4 nanocomposites at 2-18 GHz is evidently enhanced, as compared with that of both pure CNTs and CoFe2O4 nanoparticles. The enhancement mechanism is discussed based on magnetization hysteresis loop measurement and electromagnetic theory.