In this paper, a facile synthesis process is proposed to prepare multi-walled carbon nanotubes/magnetite (MWCNTs/Fe 3 O 4 ) hybrids. The process involves two steps: 1) water-soluble CNTs are synthesized by one-pot modification using potassium persulfate (KPS) as oxidant. 2) Fe 3 O 4 is assembled along the treated CNTs by employing a facile hydrothermal process with the presence of hydrazine hydrate as the mineralizer. The treated CNTs can be easily dispersed in aqueous solvent. Moreover, X-ray photoelectron spectroscopy (XPS) analysis reveals that several functional groups such as potassium carboxylate (-COOK), carbonyl (-C=O) and hydroxyl (-C-OH) groups are formed on the nanotube surfaces. The MWCNTs/Fe 3 O 4 hybrids are characterized with respect to crystal structure, morphology, element composition and magnetic property by x-ray diffraction (XRD), transmission electron microscopy (TEM), XPS and superconducting quantum interference device (SQUID) magnetometer. XRD and TEM results show that the Fe 3 O 4 nanoparticles with diameter in the range of 20-60 nm were firmly assembled on the nanotube surface. The magnetic property investigation indicated that the CNTs/Fe 3 O 4 hybrids exhibit a ferromagnetic behavior and possess a saturation magnetization of 32.2 emu/g. Further investigation indicates that the size of assembled Fe 3 O 4 nanoparticles can be turned by varying experiment factors. Moreover, a probable growth mechanism for the preparation of CNTs/Fe 3 O 4 hybrids was discussed.