Catalytic tests to assess the performance of mixed perovskite-type oxides (La0.9Ca0.1FeO3-δ, La0.6Ca0.4FeO3-δ, Nd0.9Ca0.1FeO3-δ, Nd0.6Ca0.4FeO3-δ, Nd0.6Ca0.4Fe0.9Co0.1O3-δ, Nd0.6Ca0.4Fe0.97Ni0.03O3-δ, and LSF) with respect to CO oxidation are presented as well as characterization of the materials by XRD and SEM. Perovskites are a highly versatile class of materials due to their flexible composition and their ability to incorporate dopants easily. CO oxidation is a widely used “probe reaction” for heterogeneous catalysts. In this study, it is demonstrated how tuning the composition of the catalyst material (choice of A-site cation, A-site and B-site doping) greatly influences the activity. Changing the A-site cation to Nd3+ or increasing the concentration of Ca2+ as A-site dopant improves the performance of the catalyst. Additional B-site doping (e.g., Co) affects the performance as well—in the case of Co-doping by shifting ignition temperature to lower temperatures. Thus, perovskites offer an interesting approach to intelligent catalyst design and tuning the specific properties towards desired applications.