Highly-crystalline gadolinium doped and carbon-coated ultrathin Li4Ti5O12 (LTO) nanosheets (denoted as LTO-Gd-C) as an anode material for Li-ion batteries (LIBs) are synthesized on large scale by controlling the amount of carbon precursor in the topotactic transformation of layered ultrathin Li1.81H0.19Ti2O5·xH2O (H-LTO) nanosheets at 700 °C. The characterizations of structure and morphology reveal that the gadolinium doped and carbon-coated ultrathin LTO nanosheets have high crystallinity with a thickness of about 10 nm. Gadolinium doping allows the spinel LTO products to be stabilized, thereby preserving the precursor's sheet morphology and single crystal structure. Carbon encapsulation serves dual functions by restraining crystal growth of the LTO primary nanoparticles in the LTO-Gd-C nanosheets and decreasing the external electron transport resistance. Owing to the synergistic effects rendered by ultrathin nanosheets with high crystallinity, gadolinium doping and carbon coating, the developed ultrathin LTO nanosheets possess excellent specific capacity, cycling performance, and rate capability compared with reference materials, when evaluated as an anode material for lithium ion batteries (LIBs). The simple and effective strategy encompassing nanoscale morphological engineering, surface modification, and doping improves the performance of LTO-based anode materials for high energy density and high power LIBs applied in large scale energy storage.