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A novel semiconductive Co/Fe‐MOF embedded with Fe2O3 nanocrystals (Fe2O3@CoFe‐MOF) is developed as a trifunctional electrocatalyst for the urea oxidation reaction (UOR), oxygen evolution reaction (OER), and hydrogen evolution reaction for enhancing the efficiency of the hydrogen production via the urea‐assisted overall water splitting. Fe2O3@CoFe‐TPyP‐MOF comprises unsaturated metal‐nitrogen coordination...