The hierarchical Cu2S@NC@MoS3 heterostructures have been firstly constructed by the high‐capacity MoS3 and high‐conductive N‐doped carbon to co‐decorate the Cu2S hollow nanospheres. During the heterostructure, the middle N‐doped carbon layer as the linker facilitates the uniform deposition of MoS3 and enhances the structural stability and electronic conductivity. The popular hollow/porous structures largely restrain the big volume changes of active materials. Due to the cooperative effect of three components, the new Cu2S@NC@MoS3 heterostructures with dual heterogenous interfaces and small voltage hysteresis for sodium ion storage display a high charge capacity (545 mAh g−1 for 200 cycles at 0.5 A g−1), excellent rate capability (424 mAh g−1 at 15 A g−1) and ultra‐long cyclic life (491 mAh g−1 for 2000 cycles at 3 A g−1). Except for the performance test, the reaction mechanism, kinetics analysis, and theoretical calculation have been performed to explain the reason of excellent electrochemical performance of Cu2S@NC@MoS3. The rich active sites and rapid Na+ diffusion kinetics of this ternary heterostructure is beneficial to the high efficient sodium storage. The assembled full cell matched with Na3V2(PO4)3@rGO cathode likewise displays remarkable electrochemical properties. The outstanding sodium storage performances of Cu2S@NC@MoS3 heterostructures indicate the potential applications in energy storage fields.
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