Three flexible coordination nanosheets, CoNinanosheet, Co-nanosheet, and Ni-nanosheet, were successfully synthesized using the liquid−liquid interfacial coordination method by the reaction of the ligand, 1,1,2,2-tetrakis(4-(2,2′:6′,2″-terpyridyl)phenyl)ethylene with nickel(II) and cobalt-(II) nitrates. The effective coordination between the ligand and metal ions is confirmed using characterization techniques including Fourier transform infrared spectra, X-ray photoelectron spectroscopy, scanning electron microscopy, and atomic force microscopy. The bimetallic nanosheet, CoNi-nanosheet, demonstrates an exceptional specific capacity of 112.0 mA h g −1 at 1 A g −1 . Furthermore, the CoNi-nanosheet maintains a capacity retention of 70.07% at 5 A g −1 after 1000 cycles. Upon integration into an asymmetric supercapacitor configuration, the CoNi-nanosheet assembly attains a heightened energy density of 89.0 W h kg −1 at a power density of 800 W kg −1 . Impressively, the asymmetric supercapacitor has great stability. The excellent electrochemical performance of the bimetallic CoNi-nanosheet is likely attributed to alterations of electron densities around Co 2+ and Ni 2+ ions.