Improving the performance of metal-organic framework (MOF)-based electrode materials remains a significant challenge due to their inherent instability and poor electrical conductivity. In this study, we report the development of a novel MnNi2S4-MOF-67 composite, incorporating graphene oxide (GO) and ZIF-67 as both a structural template and precursor. The synergistic effect of GO and ZIF-67 enhances the specific surface area, introduces abundant active sites for redox reactions, and shortens ion diffusion pathways. As a result, the MnNi2S4-MOF-67 composite exhibits outstanding electrochemical performance, delivering a remarkable specific capacitance of 1940 F g(-)(1) at 1 A g(-)(1). Furthermore, the material demonstrates excellent cycling stability, retaining 91% of its initial capacitance after 10,000 charge-discharge cycles at 5 A g(-)(1). When assembled into an asymmetric supercapacitor (ASC) with MnNi2S4-MOF-67@rGO//GO electrodes, the device achieves an impressive energy density of 45.90 Wh kg(-)(1) at a power density of 1689 W kg(-)(1). These results highlight the potential of hybrid-structured electrodes in advancing next-generation high-energy-density asymmetric supercapacitors.