Designing metal hydroxide electrocatalysts with high efficiency to overcome the slow reaction kinetics of the oxygen evolution reaction (OER) is considered as a significant approach for renewable energy resources. We report here a simple methodology to synthesize 2D thin nickel hydroxide/nickel oxyhydroxide sheets that show efficient activity towards OER. Further, by doping with a heteroatom, Fe, thinner sheets of nickel hydroxide/nickel oxyhydroxide are developed, which exhibit enhanced electrocatalytic activity towards OER with high durability. Fe‐doped Ni(OH)2/NiOOH requires only 200 mV overpotential to produce 10 mA/cm2, whereas bare Ni(OH)2/NiOOH needs 290 mV overpotential. Moreover, Fe‐doped nickel hydroxide/nickel oxyhydroxide shows a minimal Tafel value of 48 mV/decade, which is even lower than RuO2/CC (82 mV/decade). X‐ray photoelectron spectroscopy indicates that in the case of Fe‐doped Ni(OH)2/NiOOH, the Ni3+ signal enhances, which indicates the favourable stabilization of Ni3+ in the presence of Fe3+ dopant. Under electrochemical OER conditions, in Fe‐doped Ni(OH)2/NiOOH, Fe3+ species help to generate more Ni3+, which function as the active species. Fe0.06Ni0.94(OH)2/NiOOH shows long‐term stability for at least 24 hours in alkaline medium. This work unveils a green strategy for Fe‐doping in 2D thin sheets of Ni(OH)2/NiOOH, which show improved electrocatalytic activity compared to bare Ni(OH)2/NiOOH. The mechanism of OER activity enhancement after Fe‐doping is proposed here.