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A silicon-graphene heterostructure provides optimalelectrochemical performance as anode nanomaterial in both half andfull cells with a commercial NMC111 (LiNi1/3Mn1/3Co1/3O2) cathode.The anode consists of carbon-coated polycrystalline silicon nano-particles in between a parallel oriented few-layers grapheneflakes(FLG). Electrochemical tests in lithium cells display high capacityvalues (?2300 mAh/g) with a Coulombic efficiency (CE) reaching99% at current density of 350 mA/g and 1000 mAh/g at currentdensity values up to 3.5 A/g (CE = 99%). The laminated graphene-based structure yields a protective coating to the siliconnanoparticles still enabling exposure to lithium ions. The method of production of the laminated silicon-graphenenanocomposite is scalable and low-cost, offering a practical route to the introduction of high silicon content anodes in lithium-ion batteries.