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• The method of synthesizing the composite has been novel and has not been reported so far. • MoS 2 @Ni-MOF shows the remarkable specific capacitance. • The introduction of sulfur has established a bridge for the charge transfer. • The MoS 2 @Ni-MOF//AC ASC device exhibits a high energy density of 72.93 Wh kg−1 at power density of 375 W·kg−1. • The assembled all-solid-state MoS 2 @Ni-MOF//AC can illuminate commercial red LED lamps for up to 30 s. Two-dimensional metal-organic frameworks and nanoflowers of the MoS 2 form a composite structure as an electrode material for high-performance supercapacitor application. MoS 2 expands in the accordion-type Ni-MOF layers, and -S- joins the two materials to form a Ni-MOF coating MoS 2 composite structure. The composite material MoS 2 @Ni-MOF combines the structural characteristics of the Ni-MOF and MoS 2 , and effectively improves the electrochemical performance. The basic skeleton structure of the MoS 2 @Ni-MOF material remains unchanged, showing a remarkable specific capacitance of 1590.24 F·g−1 at a current density of 1.0 A·g−1 and an excellent cycle stability (retention rate of 87.97% after 20,000 cycles at current of 5.0 A·g−1). Due to the special composite structure of MoS 2 @Ni-MOF, the as-assembled MoS 2 @Ni-MOF//AC assymmetric supercapacitor (ASC) device exhibits a maximum energy density of 72.93 Wh·kg−1 at a power density of 375 W·Kg−1. These excellent electrochemical properties indicate that the MoS 2 @Ni-MOF has potential applications in energy storage devices. [ABSTRACT FROM AUTHOR]