The challenge to develop a highly efficient and affordable electrocatalyst for the oxygen evolution reaction (OER) could be fulfilled by a newly developed transition metal boron amorphous alloy electrocatalyst. This could successfully improve the overall efficiency of the electrochemical water splitting. Herein, we demonstrate the development of an entirely new Cu−Co−B amorphous alloy nanosheet (NS), which can act as an industrially promising electrocatalyst for the OER. Among a series of studied compositions, surface activated CuCo 2 B NSs with 5−6 nm thickness offer highly promising OER performances with an exceptionally high current density of 1000 mA cm −2 at 270 mV of overpotential (η) in a 1.0 M KOH electrolyte. It can also afford η 100 = 204 mV and η 500 = 256 mV, which remains intact for 60 h, with the lowest Tafel slope and charge transfer resistance and the highest electrochemically active sites with a promising turnover frequency and 87% Faradaic efficiency. It also fulfills the commercial requirement criteria of the OER process in 30 wt % KOH. Extensive experimental analyses led to a Cu−Co synergistic-based mechanism by the in situ formed active sites for the adsorption of *OH and *OOH reaction species, reconstruction of the catalyst surface by forming a metal hydroxides/oxyhydroxides precatalyst, modulation of electronic structure due to the rich defect nature, and topological disorder of the amorphous catalyst. Density functional theory (DFT) studies reveal that CuCo 2 B NSs are the most promising candidates for OER due to the lowest barrier for OER and thus the lowest adsorption energies, and the Cu-centers effectively and synergistically enhance the OER.