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Abstract The practical application of Fe 3 C‐based catalysts is hindered by two major challenges: the continuous dissolution of Fe atoms and the strong adsorption of oxygen intermediates. To overcome these limitations, a novel rare earth (RE) oxide/iron carbide heterostructure is designed, featuring abundant active CeO 2 /Fe 3 C interfacial sites anchored on N‐doped carbon substrates (CeO 2 /Fe 3 C@N‐C). The CeO 2 /Fe 3 C@N‐C catalyst exhibits exceptional alkaline oxygen reduction reaction (ORR) performance, with a half‐wave potential ( E 1/2 ) of 0.926 V and remarkable durability, sustaining over 20 000 cycles with minimal degradation. These metrics surpass those of commercial 20% Pt/C and most reported Fe 3 C‐based electrocatalysts. When applied as a cathode catalyst in Zn–air batteries (ZABs), CeO 2 /Fe 3 C@N‐C achieves a high‐power density of 204 mW cm⁻ 2 , demonstrating its practical potential. Through a combination of experimental characterization and density functional theory (DFT) calculations, the mechanistic origins of enhanced performance is uncovered. CeO 2 acts as an electron donor, inducing electron redistribution at the CeO 2 /Fe 3 C interface and resulting in electron accumulation at the Fe active sites. This work not only demonstrates a high‐performance ORR catalyst but also provides fundamental insights into the role of RE oxides in enhancing Fe 3 C‐based electrocatalysts. The findings offer a strategic pathway for designing advanced energy conversion materials with improved activity, stability, and efficiency.
Wang et al. (Tue,) studied this question.