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Co2V2O7/graphene composites were synthesized for lithium-ion battery (LIBs) anodes in a facile water-bath approach. The hexagonal Co2V2O7microplatelets attached uniformly to the few-layer graphene. As an unique hybrid architecture, Co2V2O7/graphene composites displayed an outstanding reversible capacity of 1048 mA h g–1at a current density of 1 A g–1over 300 cycles. The composite also demonstrated superior rate capability (∼600 mA h g–1at 2 A g–1) because of the suppression of volume expansion and the improved electrical conductivity by graphene, which was corroborated by the theoretical calculations using the density function theory. Because of the synergistic effects of graphene and Co2V2O7, the composite exhibited substantial potential as a next-generation anode material for LIBs.