The hierarchical Li4Ti5O12/C microspheres based on the waste biomass of phoenix tree leaf are synthesized as anodes for lithium-ion batteries. The phoenix tree leaf derived activated carbon (CPTL) are uniformly coated on the surface of acanthosphere-like Li4Ti5O12 (LTO) microspheres using a facial hydrothermal method to fabricate hierarchical porous structures with conducive interconnected 3D networks. Results show that the LTO-CPTL composite with 3 wt% carbon delivers the best electrochemical performance at both ambient and low temperatures with an initial discharge capacity of 212 mAh g(-1) at 1 C and capacity retention of 95% after 500 cycles. The present study demonstrates a facile and cost-efficient way to fabricate high performance electrode materials for batteries.