The oxygen evolution reaction (OER) plays a key role in determining the performance of overall water splitting, while a core technological consideration is the development of cost-effective, efficient, and durable catalysts. Here, we demonstrate a robust reduced Fe-oxide@ NiCo 2 O 4 bilayered non-precious-metal oxide composite as a highly efficient OER catalyst in an alkaline medium. A bilayered oxide composite film with an interconnected nanoflake morphology (Fe 2 O 3 @NiCo 2 O 4 ) is reduced in an aqueous NaBH 4 solution, which results in a mosslike Fe 3 O 4 @NiCo 2 O 4 (reduced Fe-oxide@NiCo 2 O 4 ; rFNCO) nanostructured film with an enhanced electrochemical surface area. The rFNCO film demonstrates an outstanding OER activity with an extraordinary low overpotential of 189 mV at 10 mA cm −2 (246 mV at 100 mA cm −2 ) and a remarkably small Tafel slope of 32 mV dec −1 . The film also shows excellent durability for more than 50 h of continuous operation, even at 100 mA cm −2 . Furthermore, density functional theory calculations suggest that the unintentionally in situ doped Ni during the reduction reaction possibly improves the OER performance of the rFNCO catalyst shifting d-band centers of both Fe and Ni active sites. KEYWORDS: bilayered Fe 3 O 4 /NiCo 2 O 4 , chemical reduction, metal interdiffusion, electrocatalytic water splitting, oxygen evolution reaction (OER)