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Two-dimensional ultrathin nickel hydroxide nanosheets with large surface area and excellent electronicproperties have been considered as promising electrocatalysts for the oxygen evolution reaction (OER). Herein, we report afacile microwave synthetic strategy to prepare ultrathin nickel hydroxide nanosheets with thickness <1 nm. In addition, varyingthe iron incorporation into the parent nickel hydroxide nanosheets allows us to synthesize a series of Ni1?xFex(OH)2nanosheetswithout sacrificing the atomic thickness. Electrochemical studies demonstrate that Fe0.22Ni0.78(OH)2nanosheets exhibit the bestOER activity, requiring an overpotential of only 315 mV to achieve 10 mA/cm2plus strong robustness in 1.0 M KOH. Theenhanced OER performance could be mainly attributed to the intrinsically more active sites in Fe0.22Ni0.78(OH)2. Overall, ourwork presents a novel and facile approach to obtain ultrathin nanosheets of nickel/iron hydroxides as competent OERelectrocatalysts. The microwave synthetic approach could be readily extended to prepare many other ultrathin oxides/hydroxides for various applications.