Three-dimensional Zn3V2O7(OH)(2)center dot 2H(2)O microspheres have been successfully synthesized by a simple and facile liquid phase precipitation method without using any surfactants or additives. The as-prepared microspheres were constructed by two-dimensional nanosheets, which interconnected with each other through self-assembly. The influences of the aging time, reaction temperature, and pH value on the morphologies of the products were systematically investigated. Moreover, three-dimensional Zn-3(VO4)(2) microspheres could be formed through calcination of the Zn3V2O7(OH)(2)center dot 2H(2)O precursor. The obtained Zn3V2O7(OH)(2)center dot 2H(2)O and Zn-3(VO4)(2) microspheres were further investigated as the anode materials of lithium-ion batteries. Electrochemical measurements showed that the Zn3V2O7(OH)(2)center dot 2H(2)O and Zn-3(VO4)(2) microspheres exhibited high discharge capacity and good cycle stability, indicating potential anode candidates in advanced rechargeable lithium-ion batteries. It should be noted that this is the first report on the Zn3V2O7(OH)(2)center dot 2H(2)O and Zn-3(VO4)(2) three-dimensional microspheres as anode materials in lithium-ion batteries. The present work will greatly expand the range of anode choices and could assist long-term endeavors in developing high capacity anode materials for lithium-ion batteries.