MoS2/RGO/Ni3S2 nanocomposite with a unique nanosheet-on-nanosheet structure was prepared through a hydrothermal process by depositing a MoS2 layer on the upper surface side of reduced graphene oxide (RGO) nanosheets and Ni3S2 layer on the lower surface sides. Furthermore, this, MoS2/RGO/Ni3S2 nanocomposite was simultaneously loaded on a Ni foam (NF) substrate. During the synthesis process, nickel foam serves not only as a support but also as the Ni source for the composite and a reductant of GO. When used as an electrochemical electrode, as-prepared MoS2/RGO/Ni3S2@NF, it exhibited excellent electrochemical performance with a high capacity of 8.841Fcm−2 at 50mAcm−2, and excellent cyclability, exhibiting capacity retention of 98.4% after 11,000 charge-discharge cycles at the current density of 80mAcm−2.