Thin iron films grown on carbon fibers were prepared by atmospheric pressure (AP), metal-organic (MO) CVD, which was conducted under pure hydrogen/argon atmospheres. Their crystalline structures and morphologies were characterized by X-ray diffraction (XRD) and scanning electron microscopy (SEM), respectively. The film growth and structure, as a function of the deposition temperature, hydrogen gas flow rate, and precursor sublimation rate, were investigated. It was concluded that the optimum control of the three above mentioned process parameters was important and essential for obtaining highquality iron film. Based on these analyses and results, a possible deposition mechanism was proposed.