We report an experimental study of the bimagnetic nanocomposites CoFe2/CoFe2O4. The precursor material, CoFe2O4 was prepared using the conventional stoichiometric combustion method. The nano-structured material CoFe2/CoFe2O4 was obtained by total oxygen reduction of CoFe2O4 using a thermal treatment at 350 °C in H2 atmospheres following the partial oxidation in O2 atmospheres at 380 °C during 120; 30; 15, 10, and 5 min. The X-ray diffraction, Mössbauer spectroscopy and transmission electronic microscopy images confirmed the formation of the material CoFe2/CoFe2O4. The magnetic hysteresis for the nanocomposite with different saturation magnetization (from 87 to 108 emu/g) also confirms the formation of the CoFe2/CoFe2O4 with different content of CoFe2O4. Furthermore, the magnetic hysteresis curves for all samples presented a single magnetic behavior, suggesting the magnetic coupling between the phases of the nanocomposite. The effects of high energy milling on the magnetic properties of the precursor material and nanocomposites samples were evaluated.