interest in mixed transition metal oxides (MTMOs). Our recent study [6] and those of others [7,8] have shown that surface defects of catalysts, particularly surface oxygen vacancies, play an important role in catalytic performance. Aliovalent substitution is considered to promote the creation of defects and vacancies, thus enhancing the catalytic reaction. [9,10] Conventional preparation methods using wet impregnation, [11,12] combustion, [13] and co-precipitation [14] are unable to produce uniform substitution beyond 10 at.%. [15] Higher loading often triggers the formation of separate oxide phases. Moreover, hightemperature post-treatment often results in sintering and loss of surface area for MTMOs prepared by these methods.Metal-organic frameworks (MOFs) were first used as catalyst precursor in making electrocatalysts. [16][17][18] More recently, ZIF-67 was used to prepare CeO 2 -doped Co 3 O 4 to catalyze the reaction of NO and CO. [19] Zamaro et al. [20] pyrolyzed the wet-impregnated Ce(III) on HKUST-1 to obtain CuO/ CeO 2 catalyst for CO oxidation. Similarly, Li and co-workers [21] calcined Cu 2+ supported on Ce-based UiO-66 to obtain CuO/ CeO 2 active for CO oxidation at around 100 °C. The degree of heterometal substitution into metal oxide lattices is limited for these examples. This work proposes a novel synthesis approach Mixed transition metal oxides (MTMOs) have enormous potential applications in energy and environment. Their use as catalysts for the treatment of environmental pollution requires further enhancement in activity and stability. This work presents a new synthesis approach that is both convenient and effective in preparing binary metal oxide catalysts (CeCuO x ) with excellent activity by achieving molecular-level mixing to promote aliovalent substitution. It also allows a single, pure MTMO to be prepared for enhanced stability under reaction by using a bimetallic metal-organic framework (MOF) as the catalyst precursor. This approach also enables the direct manipulation of the shape and form of the MTMO catalyst by controlling the crystallization and growth of the MOF precursor. A 2D CeCuO x catalyst is investigated for the oxidation reactions of methanol, acetone, toluene, and o-xylene. The catalyst can catalyze the complete reactions of these molecules into CO 2 at temperatures below 200 °C, representing a significant improvement in performance. Furthermore, the catalyst can tolerate high moisture content without deactivation.Transition metal oxides are used in many technological products in the energy and environmental fields including catalysts, [1,2] sensors, [3,4] and electrodes. [5] Being less expensive than noble metals, transition metal oxides are attractive as environmental catalysts, but reactivity and selectivity remain major hurdles. Studies show that doping and lattice substitution can enhance the catalytic activities, thus explains the growing Small 2019, 15, 1903525 1903525 (2 of 7) www.advancedsciencenews.com