Carbon nanotube-spinel lithium titanate (CNT-Li4Ti 5O12) nanoparticles have been synthesized by hydrothermal reaction and higher-temperature calcinations with LiOH-H2O and TiO2 precursors in the presence of carbon nanotubes sources. The CNT-Li4Ti5O12 nanoparticles have been characterized by X-ray diffraction (XRD), high angle annular dark field (HAADF) images, and selected area electron diffraction (SAED). The particles exhibited a spinel cubic crystal phase and homogenous size distribution, with sizes around 50-70 nm. HAADF imaging confirmed that carbon content exists on the surface of the CNT-Li4Ti5O12 nanoparticles with graphitic carbon coating of 3-5 nm thickness under 800°C in the Ar gas. The graphitic carbon phase was further confirmed with Raman spectroscopy analysis on powder samples. Electrochemical characteristics were evaluated with galvanostatic discharge/charge tests, which showed that the initial discharge capacity is 172 mA-h/g at 0.1C. The nanoscale carbon layers uniformly coated the particles, and the interconnected carbon nanotube network is responsible for the improved charge rate capability and conductivity.