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DOI: 10.1002/adma. 201404611 appropriate structures. Here, we fulfill this purpose by concentrating on intrinsic materials scope and fabricating a novel composite with MnCO 3 submicrometer-particles uniformly grafted on large-area graphene (LG, tens of micrometers in length and width). We have demonstrated that LG induces faceto-face self-assembly during ordinary electrode preparation and forms alternating layers with a continuous and close-packed configuration at the electrode level. Large-area composites were achieved by means of a reactantconversion route starting from LG and MnOOH precursor. Generally, this delicately designed architecture with selfassembly into orderly packed electrodes offers several advantages as LIB anodes (Figure S1 in the Supporting Information, shows a schematic illustration). First, LG offers perfect largearea support for MnCO 3 particles with uniform dispersion, allowing structural re-organization to be accommodated by the space between particles during cycling.[21, 22] Second, the continuous graphene networks existing in an ordered macroscopic electrode guarantee outstanding ion diffusion and electronic conduction, readily yielding high power delivery.[11, 23] Third, the inter-plane compact configuration of graphene domains provides sustained structural stability and high-packing-density energy storage.[13, 24, 25] Profiting from the combination of uninterrupted ion transport and effective structural stabilization, the MnCO 3-LG electrode delivered excellent electrochemical performance, and represents state-of-the-art design of high-power, high-efficiency, and low-cost anodes for next-generation …