The current research priorities about spinel lithium titanate (Li4Ti5O12) mainly focus on the improvement of specific capacity and rate capacity due to the intrinsic issues of Li4Ti5O12, such as low specific capacity and poor electrical conductivity, which limit the practical application of Li4Ti5O12 anodes in lithium-ion batteries. Herein, it is demonstrated that the Li4Ti5O12 with improved performance can be obtained by proper hierarchical structure construction and TiO2 in-situ decoration. In consequence, it delivers a high reversible specific capacity of 162.5 and 148.6mAhg−1 at 50 and 200mAg−1 after 900 and 2400 cycles, respectively. In addition, a capacity of 110.8mAhg−1 could be retained at a high rate of 20C even after 5000 cycles, exhibiting improved rate property and ultra-long life. This work may pave the way to facilely prepare advanced Li4Ti5O12-based anode materials for lithium-ion batteries.