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The excellent electrical conductivity of graphene is due to its highly‐conjugated structures. Manipulation of the electronic and mechanical properties of graphene can be achieved by controlling the destruction of its in‐sheet conjugation system. Herein, we report the preparation of CoCeSx−SA@BPMW@RGO through π‐π stacking interactions at the molecular level. In this study, sodium alginate was reacted with Co2+ and Ce3+, and the composite was loaded onto a graphene surface. The graphene sheets were prepared using a bi‐pyrene terminated molecular wire (BPMW) to avoid re‐stacking of the grapheme sheets, thereby forming nanoscale spaces between sheets. The angle between the BPMW coplanar pyrene group and the phenyl group was 33.2°, and the graphene layer is supported in an oblique direction. Finally, a three‐dimensional porous composite was obtained after annealing and vulcanization. The obtained CoCeSx−SA@BPMW@RGO exhibited excellent electrical conductivity and remarkable cycle stability. When the current density was 1 A g−1, its specific capacitance was as high as 1004 F g−1. BPMW modifies graphene through the synergistic effect of π‐π stacking interaction and special structure to obtain excellent electrochemical performance. Moreover, a solid‐state asymmetric supercapacitor device was fabricated based on the synthesized CoCeSx−SA@BPMW@RGO hybrid, which exhibited a power density of 979 W kg−1 at an energy density of 23.96 Wh kg−1. [ABSTRACT FROM AUTHOR]