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To meet current economic demands enforcing the replacement of platinum-group metals, extensively used in three-way-catalytic converters (TWC), research is driven towards low-cost and widely available base metals. However, to cope with their lower activity, high metal loadings must be coupled with increased dispersion. Herein, a series of CuO/Al₂O₃ samples is produced and the effect of different alumina supports’ properties on CuO dispersion, speciation and eventually on the TWC performance is studied. The alumina samples are synthesized via different methods, including soft-templating routes and flame spray pyrolysis, and compared with a commercial one, while CuO used as the catalytic active phase is added through ammonia-driven deposition–precipitation. As found, the large surface area and low crystallinity of the aluminas produced by soft-templating routes favor strong metal–support interaction, generating highly dispersed and strongly bonded CuO species at low loading and copper-aluminate phases at high loading. Notably, the use of amorphous mesoporous alumina completely prevents the formation of crystalline CuO even at 15 wt% Cu. Such high metal loading and dispersion capacity without the application of elevated calcination temperatures is one of the best reported for nonreducible supports. Catalytic evaluation of this material reveals a pronounced enhancement of oxidation activity with metal loading increase.