Conformal carbon-coated Li4Ti5O12 (LTO) fibers are easily synthesized through a simple electrospinning route combined with subsequent thermal treatment. The as-formed fibers comprise interconnected LTO nanoparticles and an external coating layer of carbon. When evaluated as an anode material for lithium-ion batteries, the resulting LTO/C fibers exhibit excellent high-rate lithium-storage performances. The influence of the carbon content in the composite LTO/C fibers on the electrochemical properties is explored in detail. The enhanced lithium-storage performances are attributed to the synergetic features of interconnected LTO nanocrystals and a highly electronically conductive coating layer of carbon, which reduce the Li+ -diffusion distance and improve the electronic conductivity. This work presents a facile and effective synthetic strategy, which is potentially competitive for scaling-up the industrial production of high-rate LTO anode materials for lithium-ion batteries.