In this work, the covalent attachment of an amine functionalized metal‐organic framework (UiO‐66‐NH₂ = Zr₆O₄(OH)₄(bdc‐NH₂)₆; bdc‐NH₂ = 2‐amino‐1,4‐benzenedicarboxylate) (UiO‐Universitetet i Oslo) to the basal‐plane of carboxylate functionalized graphene (graphene acid = GA) via amide bonds is reported. The resultant GA@UiO‐66‐NH₂ hybrid displayed a large specific surface area, hierarchical pores and an interconnected conductive network. The electrochemical characterizations demonstrated that the hybrid GA@UiO‐66‐NH₂ acts as an effective charge storing material with a capacitance of up to 651 F g⁻¹, significantly higher than traditional graphene‐based materials. The results suggest that the amide linkage plays a key role in the formation of a π‐conjugated structure, which facilitates charge transfer and consequently offers good capacitance and cycling stability. Furthermore, to realize the practical feasibility, an asymmetric supercapacitor using a GA@UiO‐66‐NH₂ positive electrode with Ti₃C₂T_X MXene as the opposing electrode has been constructed. The cell is able to deliver a power density of up to 16 kW kg⁻¹ and an energy density of up to 73 Wh kg⁻¹, which are comparable to several commercial devices such as Pb‐acid and Ni/MH batteries. Under an intermediate level of loading, the device retained 88% of its initial capacitance after 10 000 cycles.