In this study, spinel lithium titanate (Li4Ti5O12, LTO) anode materials were synthesized from two titanium sources (P25 TiO2, 100% anatase TiO2) using a spray-drying method and subsequent calcination at various temperatures. The electrochemical performance of both a Li/LTO half cell and a LiNi0.5Mn1.5O4/LTO (LNMO/LTO) full cell were investigated. The electrochemical performance of the LTO material prepared from P25 TiO2 was superior to that of the LTO prepared from 100% anatase TiO2. After modification of LTO material with AlPO4, the LTO coated with 2 wt% of AlPO4 (denoted “2%AlPO4-LTO”) provided the best performances. The specific (delithiation) capacities of the 2%AlPO4-LTO anode material was 189.7 mA h g−1 at 0.1C/0.1C, 184.5 mA h g−1 at 1C/1C, 178.8 mA h g−1 at 5C/5C, and 173.1 mA h g−1 at 10C/10C. From long-term cycling stability tests, the specific capacity at the first cycle and the capacity retention after cycling were 185.5 mA h g−1 and 98.06%, respectively, after 200 cycles at 1C/1C and 182.1 mA h g−1 and 99.18%, respectively, after 100 cycles at 1C/10C. For the LNMO/2%AlPO4-LTO full cell, the average specific capacity (delithiation) and coulombic efficiency after the first five cycles were 164.8 mA h g−1 and 93.30%, respectively, at 0.1C/0.1C. The specific capacities at higher C-rates were 156.1 mA h g−1 at 0.2C/0.2C, 135.7 mA h g−1 at 1C/1C, 97.5 mA h g−1 at 3C/3C, and 46.5 mA h g−1 at 5C/5C. After twenty-five cycles, the C-rate returned to 1C/1C and the specific capacity, coulombic efficiency, and capacity retention were maintained at 134.1 mA h g−1, 99.17%, and 98.82%, respectively.