Zhonglu Hu, Cong Wang, Fengqi Li, Haifeng Bian, Qing Zhou, Ge Xue, Shunshun Jia, Hailong Wu, Jian Gu, Yujie Ma, Xiangkang Meng
ABSTRACT The development of efficient, stable bifunctional electrocatalysts for sustainable hydrogen production via water electrolysis remains challenging due to the high cost and instability of precious metal catalysts. This study addresses this by constructing a heterointerfacial CoFe 2 O 4 /CeO 2 composite anchored on carbon (CoFe 2 O 4 /CeO 2 @C) through a facile hydrothermal‐pyrolysis approach. The optimized catalyst demonstrates exceptional activity, achieving overpotentials of 243 mV for oxygen evolution reaction (OER) and 82 mV for hydrogen evolution reaction (HER) at 10 mA cm −2 in 1 M KOH, significantly outperforming benchmark RuO 2 and Pt/C, alongside requiring only 1.57 V to drive overall water splitting at 10 mA cm −2 . Structural and electronic analyses confirm that the heterointerface between CoFe 2 O 4 and CeO 2 facilitates charge redistribution, thus optimizing the electronic environment. Remarkably, the catalyst demonstrated only a 6.1% decay in current density after a 24‐h stability test and exhibits high Faradaic efficiency. This work provides a scalable strategy for designing non‐precious metal bifunctional catalysts for overall water splitting.