In this work, 3D microsphere Zn2V2O7 is obtained by calcined the precursor Zn3(OH)2V2O7·2H2O. The 3D structure of Zn2V2O7 inherits from the precursor which is composed by layered structures with nanoparticles fully covered. The unique structure endows it higher specific surface area and porous structure. Benefitting from the structure stability and the synergistic effect of the mixed metal oxides, the Zn2V2O7 electrode shows high specific capacity of 84.8 mAh g−1 at 1 A g−1, good rate capability and long cycle life. In addition, the battery-supercapacitors hybrid device is assembled with Zn2V2O7 as positive electrode and AC as negative electrode. The device shows high cycling stability with 89.8% retention after 6000 cycles and maximum energy density of 34.99 Wh kg−1 at 850 W kg−1. The high specific capacity and energy density suggest that 3D Zn2V2O7 microsphere electrode material is suitable for application in the field of alkaline rechargeable battery.