MoS2 has been investigated extensively as novel energy storage materials because of its unique physical and chemical properties. Herein, a flexible Three-Dimensional (3D) free-standing composite is rationally designed and synthesized by growing MoS2 nanosheets onto carbonized melamine foam. Afterwards, nitrogen-doped carbon (NC) coating is created on the bare MoS2 nanosheets depends on dopamine self-polymerization. The composite can be used directly as a free-standing anode for lithium-ion batteries. It exhibits high reversible lithium storage capacity with good cyclic performance (573.8 mAh g(-1) at current density of 500 mA g(-1) after 200 cycles) and rate capability (536.9 mAh g(-1) at current density of 2000 mA g(-1)). The outstanding electrochemistry properties are mainly attributed to the well-designed architecture. The interconnected carbon skeleton provides 3D fast transport paths for electron. NC coating on MoS2 nanosheets and the carbon filled in the interspaces between MoS2 nanosheets serves as conductive matrix which enhances the electrical conductivity, expands the path of electron transport and accelerates electron transfer.