Transition metal oxides show great promise as high-energy anodes for lithium-ion batteries (LIBs), thanks to appealing combination of high theoretical specific capacity and low cost. However, they still undergo dramatic volumetric expansion and low electronic/ionic conductivities, which leads to numerous problems, for instance, rapid capacity degradation and electrode pulverization, thus severely hindering their practical applications. In this paper, a designed hydrangea-like microstructure consisting of MnO(2)nanosheets and ZnFe(2)O(4)microspheres is achieved by a hydrothermal route. When evaluated as an anode material for LIBs, ZnFe2O4@MnO(2)electrode displays a high specific capacity of 2707 mA h g(-1)after 100 cycles at 0.2 A g(-1). Even at a higher current density of 2 A g(-1), the electrode has a long lifespan with a specific capacity of 1458 mA h g(-1)after 800 cycles and outperforms the previously reported zinc ferrite composite electrodes. These excellent electrochemical properties are ascribed to the hydrangea-like structure, which buffers the volume variation of ZnFe(2)O(4)during charging/discharging process and decreases the internal resistance significantly due to excellent contact between ZnFe(2)O(4)microparticles and MnO(2)nanosheets. Consequently, the facile synthesis strategy and superior Li-storage performance make the hydrangea-like ZnFe2O4@MnO(2)microspheres the promising candidate for next-generation high-performance LIBs in the future.