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We report the synthesis of micro-sized silicon–carbon (Si–C) composites, which simultaneously possess primary sub-10 nm Si particles and secondary micro-sized aggregation coated with carbon. Because of this unique structure, the as-synthesized Si–C composite anode can deliver excellent cycling stability with a high reversible specific capacity (∼1600 mA h g−1) within 150 cycles at 400 mA g−1. Moreover, a high volumetric capacity of ∼1088 mA h cm−3 was demonstrated by using this composite cathode, which is 5 times higher than that of commercially available nano-silicon based anodes.