The effect of different supports (Al2O3, CeO2, MgAl2O4, SiO2, and ZrO2) on the catalytic performance of an aluminum-incorporated cobalt catalyst in the dry reforming of methane (DRM) was investigated. DRM observations revealed the highest CH4 and CO2 conversion levels with CoAl/MgAl2O4. These levels decreased in the order: CoAl/MgAl2O4 > CoAl/Al2O3 > CoAl/ZrO2 > CoAl/CeO2 > CoAl/SiO2. Due to the proximity of the Co and Mg ionic radii, the cobalt species strongly interacted with MgAl2O4 resulting in the formation of a solid solution. The CH4/CO2 thermogravimetric results indicated that the performance of the CoAl/MgAl2O4 catalyst was superior to that of the other catalysts. This was attributed to the balance between the rates of carbon deposition from CH4 decomposition and surface oxidation from CO2 dissociation. In addition, the apparent activation energy on this catalyst (54.6 kJ/mol) was much lower than that of CoAl/Al2O3 (77.5 kJ/mol), indicating a marked improvement in CH4 reforming activity for CoAl/MgAl2O4. Overall, the characterization results revealed that the catalytic performance was influenced by the synergistic effect between CoAl and its support.