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. © 2025 Elsevier B.V., All rights reserved.