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Nitrous oxide (N₂O), produced from several human activities, is considered a greenhouse gas with significant environmental impacts. The most promising abatement technology consists of the catalytic decomposition of N₂O into nitrogen and oxygen. Many recently published papers dealing with N₂O catalytic decomposition over Ni-substituted Co₃O₄ are related to the treatment of N₂O concentrations less than 2 vol% in the feed stream. The present work is focused on developing catalysts active in the presence of a gaseous stream richer in N₂O, up to 20 vol%, both as powder and in structured configurations suitable for industrial application. With this aim, different nickel-cobalt mixed oxides (Ni_xCo_1−xCo₂O₄) were prepared, characterized, and tested. Subsequently, since alumina-based slurries assure successful deposition of the catalytic species on the structured carrier, a screening was performed on three nickel-cobalt-alumina mixed oxides. As the latter samples turned out to be excellent catalysts for the N₂O decomposition reaction, the final catalytic formulation was transferred to a silicon carbide monolith. The structured catalyst led to the following very promising results: total N₂O conversion and selectivity towards N₂ and O₂ were reached at 510 °C by feeding 20 vol% of N₂O. It represents an important achievement in the view of developing a more concretely applicable catalytic system for industrial processes.