VPO4/C nanosheets and microspheres are successfully synthesized via a hydrothermal method followed by calcinations. The XRD results reveal that the obtained products both have an orthorhombic VPO4 phase. The SEM and TEM images demonstrate that nanosheets and spherical morphology can be obtained by controlling the synthesis conditions. The samples are both uniformly coated by amorphous carbon. The electrochemical test results show that the sample with a nanosheet structure has a better electrochemical performance than the microsphere samples. The VPO4/C nanosheets can deliver an initial discharge capacity of 788.7 mAh g(-1) at 0.05 C and possessed a favorable capacity at the rates of 1, 2, and 4 C. The nanosheet structure can effectively improve the electrochemical performances of VPO4/C anode materials.