A series of composites of Li4Ti5O12 particles well dispersed among graphene oxide (GO) nanosheets as binder-free anode materials for high capacity and rate lithium-ion batteries are prepared and investigated. The morphology, microstructure and elemental compositions of the as-prepared composites are characterized by scanning electron microscopy, transmission electron microscopy, X-ray diffraction and X-ray photoelectron spectroscopy. Electrochemical tests reveal that the electrode with GO content 10% presents a reversible Li-ion storage specific capacity of 201 mAh g−1 at 0.5C (1C = 175 mA g−1), and the specific capacity still maintain in 162 mAh g−1 even at 30C. Moreover, this composite exhibits an excellent cycling stability, with a first charge capacity of 162 mAh g−1 at 30C and less than 3% loss after 300 cycles. The addition of GO provides the additional capacity via oxygen-containing functional group and nano-cavity, additionally, replacing the CMC by GO, which makes the composite with CMC binder-free, speeds up the lithium ion diffusion in anode materials.