Spinel-type cobalt oxide is a highly active catalyst for oxidation reactions owing to its remarkable redox properties, although it generally exhibits poor mechanical, textural and structural properties. Supporting this material on a porous alumina can significantly improve these characteristics. However, the strong cobalt–alumina interaction leads to the formation of inactive cobalt aluminate, which limits the activity of the resulting catalysts. In this work, three different strategies for enhancing the performance of alumina-supported catalysts are examined: (i) surface protection of the alumina with magnesia prior to the deposition of the cobalt precursor, with the objective of minimizing the cobalt–alumina interaction; (ii) coprecipitation of cobalt along with nickel, with the aim of improving the redox properties of the deposited cobalt and (iii) surface protection of alumina with ceria, to provide both a barrier effect, minimizing the cobalt–alumina interaction, and a redox promoting effect on the deposited cobalt. Among the examined strategies, the addition of ceria (20 wt % Ce) prior to the deposition of cobalt resulted in being highly efficient. This sample was characterized by a notable abundance of both Co3+ and oxygen lattice species, derived from the partial inhibition of cobalt aluminate formation and the insertion of Ce4+ cations into the spinel lattice.