Because of its extreme safety and outstanding cycle life, Li 4 Ti 5 O 12 has been regarded as one of the most promising anode materials for next-generation high-power lithium-ion batteries. Nevertheless, Li 4 Ti 5 O 12 suffers from poor electronic conductivity. Here, we develop a novel strategy for the fabrication of Li 4 Ti 5 O 12 /carbon core−shell electrodes using metal oxyacetyl acetonate as titania and single-source carbon. Importantly, this novel approach is simple and general, with which we have successfully produce nanosized particles of an olivine-type LiMPO 4 (M = Fe, Mn, and Co) core with a uniform carbon shell, one of the leading cathode materials for lithium-ion batteries. Metal acetylacetonates first decompose with carbon coating the particles, which is followed by a solid state reaction in the limited reaction area inside the carbon shell to produce the LTO/C (LMPO 4 /C) core−shell nanostructure. The optimum design of the core−shell nanostructures permits fast kinetics for both transported Li + ions and electrons, enabling high-power performance. KEYWORDS: Lithium ion batteries, Li 4 Ti 5 O 12 , lithium metal phosphates, core−shell structures, anode, cathode L ithium-ion batteries (LIBs), dominating the portable power market, have attracted enormous attention in the last several years for large-scale battery applications, such as electric vehicles (EV) and hybrid electric vehicles (HEV). 1,2 However, further improvements in terms of power densities, safety, and lifetime require new materials or new structures with a higher storage capacity and faster charge and discharge rate and desired potentials. 3−6 Graphitic carbon is commonly used as an anode in commercial LIBs but exhibits poor rate performance due to its low Li diffusion coefficient and presents serious safety issues because of potential solid electrolyte interphase (SEI) film formation. 7−10 As for cathode materials, lithium transition metal oxides suffer from the intrinsic disadvantage of poor thermal stability due to the release of oxygen from the highly delithiated oxide materials. 11 Advanced materials with better safety and excellent rate capability are critical components for the next generation of LIBs.Compared to graphite, spinel Li 4 Ti 5 O 12 (LTO) exhibits a relatively high lithium insertion/extraction voltage of approximately 1.55 V (vs Li/Li + ), which circumvents the formation of the SEI and suppress lithium dendrite deposition on the surface of the anode. 12−14 As a zero-strain insertion material, LTO possesses excellent reversibility and excellent Li-ion mobility in the charge−discharge process. 15−17 As a cathode material, olivine-type LiMPO 4 (M = Fe, Mn, Co, and Ni) compounds which display high Li-ion mobility, superior safety properties, and high electrochemical and thermal stability. 18−23 Therefore, a LiMPO 4 /LTO cell system possessing unique properties would enable a promising rechargeable batteries for large-scale application.However, both materials suffer from poor electronic conductivity (for example: ...