Nanoscale coordination polymers (nCPs) have obtained significant attention as cutting-edge materials for energy storage equipment. Nevertheless, monometallic nCPs are often challenging in terms of high capacitance, tunable electrochemical activity, and high conductivity. Herein, an available strategy for boosting the electroconductibility and structure stability of Ni-based nCPs is presented by partially substituting Ni 2+ with proper level Co 2+ stoichiometry. Co 2+ has a beneficial effect on the electrochemical behavior of Ni/Co-nCPs. The bimetallic Ni/Co-nCPs with an appropriate ratio of Ni/Co being 4 has a high C s of 1160.2 F g −1 , which is about 1.47-fold that of Ni-nCPs. When Ni/Co-nCPs are applied as the anode in an asymmetric supercapacitor, the device gives rise to an exceptional energy density of 43.7 W h kg −1 at a power density of 594.9 W kg −1 and a remarkable capacitance retention over 7000 cycles. The strategy established in this work paves a pathway for the rational design and facile preparation of bimetallic Ni/Co-nCPs for energy storage devices with boosting electrochemical properties.