Metal‐organic frameworks (MOFs), as high‐potential electrode materials for applications in supercapacitors, have received significant attention recently. Unfortunately, MOF materials still suffer from unsatisfactory specific capacitances due to poor conductivity and limited redox active sites. In this work, a novel cobalt‐copper‐based bimetal–organic framework (CoCu‐MOF) was synthesized by a bottom‐up synthesis strategy, the material properties systematically characterized, and finally investigated as a supercapacitor electrode material. The synthesized CoCu‐MOF presented a high specific surface area of 62.4 m2 g−1, and 83% of the copper ions attained the +1 oxidation state contributing to the formation of additional redox active sites and leading to the formation of dual‐redox sites. The CoCu‐MOF displayed an excellent specific capacitance of 618 F g−1 at a current density of 1 A g−1, which was more than twice that of Co‐MOF and four times that of Cu‐MOF. The CoCu‐MOF retained 75% of its original capacitance after 3000 charge‐discharge cycles at the current density of 1 A g−1. Overall, this work demonstrates how the bimetallic synergistic strategy can effectively enhance the electrochemical properties of MOFs by providing a higher specific surface area and by the introduction of dual redox sites.This article is protected by copyright. All rights reserved.