A cross-linked MnO2 coated ZnFe2O4 hollow nanosphere composite is synthesized and controlled via a facial and handy route. The connected MnO2 nanoplates form a cross-linked network, which is conducive to the rapid transfer of Li ions. The composite with unique architecture can not only release the strain and stress caused by the insertion and desertion of lithium ions but also greatly improve the electrical conductivity and lithium ion diffusivity. Consequently, when used as a lithium-ion battery anode material, the electrode shows an excellent initial reversible capacity of 933.5 mAh/g with an initial coulombic efficiency of 62.5%. After 100 cycles, the reversible capacity stabilized at 605.6 mAh/g with a high capacity retention of 91% from the 20th cycle to the 100th cycle. At a high current density of 3 A/g, an excellent capacity of 390.6 mAh/g can be retained. In this case, the electrode shows broad application prospects for novel power storage systems.