Vanadium oxy-acetylacetonate (VO(acac)(2)) was originally explored as an organic anode material for lithium-ion batteries (LIBs) with high capacity and rate performance. Specifically, the prepared VO(acac)(2) has delivered capacity of 620 mA h g(-1) at current density of 100 mA g(-1) with nearly 100% coulombic efficiency during cycling. Furthermore, the cell exhibits good ultralong cycle stability and performs capacity of 508.5 mA h g(-1) after 1000 cycles under 1000 mA g(-1). Therefore, in the absence of any structure manipulation or conductive additives, the pristine VO(acac)(2) shows high promises as advanced anode candidate of high capacity for LIBs.