Co6Al2HT hydrotalcite-like compounds were synthesized by three different methods: co-precipitation, microwaves-assisted and ultrasound-assisted methods. The mixed oxides obtained after calcination were studied by several techniques: XRD, TEM, H2-TPR and XPS. They were also tested as catalysts in the reaction of total oxidation of toluene. The physico-chemical studies revealed a modification of the structural characteristics (surface area, morphology) as well as of the reducibility of the formed mixed oxides. The solid prepared by microwaves-assisted synthesis was the most active. Furthermore, a relationship between the ratio of Co2+ on the surface, the reducibility of the Co-Al mixed oxide and the T50 in toluene oxidation was demonstrated. This suggests a Mars Van Krevelen mechanism for toluene total oxidation on these catalysts.