Three kinds of carbon materials, i.e., graphene sheets (GSs), expanded graphite (EG) and natural graphite (NG) were comparatively investigated as anode materials for lithium-ion batteries via scanning electron microscope, high-resolution transmission electron microscopy, X-ray diffraction, Fourier transform infrared spectroscopy, Raman spectroscopy and a variety of electrochemical testing techniques. The test results showed that the reversible capacities of GS electrode were 1130 and 636mAhg−1 at the current densities of 0.2 and 1mAcm−2, respectively, which were almost twice those of EG electrode and three times those of NG electrode. The first-cycle coulombic efficiency and capacity retention of NG were much bigger than those of GSs and EG. The notable capacity fading observed in GSs and EG may be ascribed to the disorder-induced structure instability. The larger voltage hysteresis in GS and EG electrodes was not only related to the surface functional groups, but also to the active defects in GSs and EG, which results in greater hindrance and higher overvoltage during lithium extraction from electrode. The kinetics properties of GSs, EG and NG electrodes were compared by AC impedance measurements. GS and EG electrodes exhibited higher electrochemical activity and more favorable kinetic properties during charge and discharge process.