Anisotropically grown Li 3 V 2 (PO 4 ) 3 nanocrystals, which are highly dispersed and directly impregnated on the surface of a carbon nanofiber (CNF), were successfully synthesized via a two-step synthesis process: i) precipitation of nanoplated V 2 O 3 precursors (20-200 nm); ii) transformation of the V 2 O 3 precursor into Li 3 V 2 (PO 4 ) 3 nanoplates without size change. The direct attachment of the Li 3 V 2 (PO 4 ) 3 nanocrystals to the carbon surface improves the electronic conductivity and Li + diffusivity of the entire Li 3 V 2 (PO 4 ) 3 /CNF composite, simultaneously producing a mesoporous network (pore size of approximately 10 nm) that acts as an electrolyte reservoir owing to the pillar effect of the impregnated Li 3 V 2 (PO 4 ) 3 crystals. This ideal Li 3 V 2 (PO 4 ) 3 /CNF nanostructure enabled a 480C rate (7.5 seconds) discharge with 83 mA h g −1 , and 69% of capacity retention at the slowest discharge rate (1C). Such an ultrafast charge-discharge performance opens the possibility of using Li 3 V 2 (PO 4 ) 3 as a cathode material for ultrafast lithium ion batteries with a stable cycle performance over 10,000 cycles at a 10C rate, maintaining 85% of the initial capacity. In the current society, the storage of electrical energy at high charge and discharge rate is an important technological issue as it enables hybrid and plug-in hybrid electric vehicles and provides a back-up to wind and solar energies.1,2 Rechargeable lithium-ion batteries (LIBs) are considered the most advanced energy storage systems; they possess high energy but limited power compared to high-power devices such as supercapacitors.1 To further improve the performance of the LIBs, several electrode materials have been proposed and investigated so far.2-11 Commercial cells utilize the layer-structured LiCoO 2 as the positive electrode, 3 but the high cost and toxicity of cobalt prohibit its use on a large scale. Spinel-type LiMn 2 O 4 is one of the alternative materials to cobalt for high-rate use. 4 Several reports on such materials for high-rate use have been published; however, the reported discharge performance are limited within 50-150C. Owing to their easy release of oxygen, LiCoO 2 and LiMn 2 O 4 also have safety issues at overcharged states or high temperatures.3,4 Thus, to achieve a long-term and safe use of the LIBs, cathode materials other than those including layer-structured or spinel-type materials have received significant attention. Researchers have identified polyanion-type cathode materials-such as phosphate cathode materials like LiFePO 4 (LFP) 5 and Li 3 V 2 (PO 4 ) 3 (LVP)-as attractive active materials because of their high thermal stability, high cyclability, and superior safety properties provided by the stable (PO 4 ) 3− unit. 6 The presence of a phosphate with a strong P-O covalency stabilizes the antibonding M-O (M = V or Fe) energy level through an M-O-P inductive effect and generates a conveniently high redox potential for M 3+ /M 2+ . 7 In particular, monoclinic LVP has attracted much attention because o...