Lightweight and flexible electromagnetic interference (EMI) shielding materials are in great demand for wearable EMI device. In the present work, lightweight and flexible carbon nanotube (CNT)/ferroferric oxide ( Fe3O4) composite film was made through a feasible chemical vapor deposition process for CNT film synthesis, followed by a hydrothermal reduction process for Fe3O4 coating. In the as-prepared composite, CNT film and Fe3O4 particles work as conductive skeleton and strong magnetic particle, respectively. The as-prepared composite film shows a novel EMI shielding effectiveness (SE) of 91 dB in the X-band, a small thickness of 0.09 mm and a low density of 0.86 g/cm3, which is superior to most of the carbonbased EMI materials.