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A novel Layered@Spinel@Carbon heterostructure is successfully fabricated via an in situ synchronous carbonization-reduction process based on a bio-inspired coating method, which comprises a core of Li-rich layered (Rm) oxide, a spinel phase (Fdm) interlayer and a carbon nano-coating. This unique structure, which combines the advantages of the high capacity Li-rich layered structure, 3D fast Li+ diffusion channels of the spinel structure and the high conductivity of the carbon coating, shows extremely high discharge capacity (as high as 334.5 mA h g−1) and superior rate capability. This strategy may provide some new insights into the design and synthesis of various electrode materials for high performance energy storage devices.