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The development of highly efficient electrocatalysts for complete oxidation of ethylene glycol (EG) in direct EG fuel cells is of decisive importance to hold higher energy efficiency. Despite some achievements, their progress, especially electrocatalytic selectivity to complete oxidated C1 products, is remarkably slower than expected. In this work, we developed a facile aqueous synthesis of Ir‐doped CuPd single‐crystalline mesoporous nanotetrahedrons (Ir‐CuPd SMTs) as high‐performance electrocatalyst for promoting oxidation cleavage of C−C bond in alkaline EG oxidation reaction (EGOR) electrocatalysis. The synthesis relied on precise reduction/co‐nucleation and epitaxial growth of Ir, Cu and Pd precursors with cetyltrimethylammonium chloride as the mesopore‐forming surfactant and extra Br− as the facet‐selective agent under ambient conditions. The products featured concave nanotetrahedron morphology enclosed by well‐defined (111) facets, single‐crystalline and mesoporous structure radiated from the center, and uniform elemental composition without any phase separation. Ir‐CuPd SMTs disclosed remarkably enhanced electrocatalytic activity and excellent stability as well as superior selectivity of C1 products for alkaline EGOR electrocatalysis. Detailed mechanism studies demonstrated that performance improvement came from structural and compositional synergies, which kinetically accelerated transports of electrons/reactants within active sites of penetrated mesopores and facilitated oxidation cleavage of high‐energy‐barrier C−C bond of EG for desired C1 products. More interestingly, Ir‐CuPd SMTs performed well in coupled electrocatalysis of anode EGOR and cathode nitrate reduction, highlighting its high potential as bifunctional electrocatalyst in various applications. [ABSTRACT FROM AUTHOR]