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A fast one‐step arc discharge exfoliation method is employed to synthesize Si/graphene composites by using a graphite rod filled with a mixture of Si powder and urea as a cathode. During the arc discharge process, the use of urea allows both the introduction of nitrogen atoms into the graphene and the uniform sealing of Si nanoparticles between the thin graphene sheets to occur simultaneously. The resulting N‐doped graphene nanosheets embedded with Si (Si@NG) can act as an electrode material for lithium‐ion batteries and delivers the reversible capacity of 1030 mAh g−1 with a current density of 200 mA g−1 over 100 cycles along with an outstanding coulombic efficiency of 96.84 %. The remarkable electrochemical rate capability performance can be owed to the multiple role of NG, which not only serves as a three‐dimensional conductive support, but also effectively limits the volume variation of Si nanoparticles. The approach proposed here is expected to be extended to the preparation of other alloy anode/graphene hybrids for lithium ion batteries. [ABSTRACT FROM AUTHOR]