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A well-organized flexible interleaved composite of graphene nanosheets (GNSs) decorated with Fe₃O₄ particles was synthesized through in situ reduction of iron hydroxide between GNSs. The GNS/Fe₃O₄ composite shows a reversible specific capacity approaching 1026 mA h g⁻¹ after 30 cycles at 35 mA g⁻¹ and 580 mAh g⁻¹ after 100 cycles at 700 mA g⁻¹as well as improved cyclic stability and excellent rate capability. The multifunctional features of the GNS/Fe₃O₄ composite are considered as follows: (i) GNSs play a “flexible confinement” function to enwrap Fe₃O₄ particles, which can compensate for the volume change of Fe₃O₄ and prevent the detachment and agglomeration of pulverized Fe₃O₄, thus extending the cycling life of the electrode; (ii) GNSs provide a large contact surface for individual dispersion of well-adhered Fe₃O₄ particles and act as an excellent conductive agent to provide a highway for …