Li4Ti5O12 nanoclusters are successfully prepared by a facile solution-based method and subsequent calcination. The influences of calcination temperatures on the microstructure and electrochemical performance of the products are studied. Results indicate that the sample annealed at 700°C exhibits outstanding rate performances and excellent long-term cycle stabilities. It displays a high initial Coulombic efficiency of 96.0% and a desirable discharge capacity of 176mAhg−1 at 0.1°C between 1.0 and 2.5V (vs. Li/Li+). The discharge capacity at 10°C is as high as 116mAhg−1 with capacity retention of 95.7% over 100cycles. Therefore, this Li4Ti5O12 nanocluster material can be a superior and practical candidate for the anodes of high-power lithium-ion batteries.