The commercial Li4Ti5O12 (LTO) is successfully modified by AlF3 via a low temperature process. After being calcined at 400 °C for 5 h, AlF3 reacts with LTO to form a composite material which mainly consists of Al3+ and F− co-doped LTO with small amounts of anatase TiO2. Al3+ and F− co-doped LTO demonstrates ultrahigh rate capability comparing to the pristine LTO. Since the amount of the byproduct TiO2 is relatively small, the modified LTO electrodes retain the main voltage characteristics of LTO with a minor feature similar to those of anatase TiO2. The doped LTO anodes deliver slightly higher discharge capacity and maintain the excellent long-term cycling stability when compared to the pristine LTO anode. Therefore, Al3+ and F− co-doped LTO composite material synthesized at low temperature is an excellent anode for stable and ultra-high power lithium-ion batteries.