A novel heterostructured cathode material, comprised of a core of Li-rich layered (Rm) oxides integrated with Li⁺-conductive Li₂SiO₃ and an in situ formed spinel (Fdm) nano-coating layer, has been successfully synthesized. The ionic conductor Li₂SiO₃ in the bulk facilitates the Li⁺ intercalation/deintercalation process and stabilizes the layered structure. This is coupled with the fast 3D Li⁺ diffusion channels of an electrochemically active spinel coating layer, leading to superior rate capability (94 mA h g⁻¹ at 10C) and excellent cycling stability in the heterostructured cathode material. This synergistic strategy may provide some new directions for synthesizing high-performance Li-ion battery cathode materials.