The synthesis of nanostructured transition metal compounds with adjustable components are often challenging due to the involvement of multiple synthetic procedures or complex manipulations. In this work, a one-step self-regulating acid-etching strategy is employed for nickel iron-layered double hydroxide (NiFe LDH). A two-dimensional (2D) NiFe LDH nanosheet is speedy and efficiently formed. This as-prepared NiFe LDH exhibits electrocatalytic activity for oxygen evolution reaction (OER). This approach avoids numerous structural design challenges and provides highly active sites and a robust interface between catalyst and support. As a result, 2D NiFe LDH electrodes demonstrate highly efficient OER performance with a low overpotential of 300 mV and a Tafel slope of 70.6 mV dec−1 at a current density of 100 mA cm−2.