In this study, a series of hydrotalcite-derived oxides MAlO (M = Mn, Co, Ni, Fe) were prepared by calcinating of hydrotalcite for acetone and acetaldehyde total oxidation. Detailed results confirmed that the highest of CO2 yield and the lowest amount of by-product was observed over MnAlO catalyst. In particular, the MnAlO catalyst appeared to have the best catalytic performance for acetone and acetaldehyde oxidation with T-100 about 170 degrees C and 150 degrees C at a high space velocity, respectively. Catalytic activity was significantly governed by the excellent reducibility (Mn4+/Mn3+) and abundant chemical adsorption oxygen species (Oadsorbe/Olattice) of the catalysts. Besides, acid property of catalysts was beneficial to catalytic oxidation process. Interestingly, the lower amounts of by-product (acetaldehyde) were generated for acetone oxidation over MnAlO than those of other catalysts, it did not influence on the total oxidation of acetone due to its superior catalytic activity, it was investigated and analyzed the reaction mechanism of acetone oxidation and the formation of by-product over MnAlO catalyst, the result confirmed that desorption of reactant molecule and negative effect of water vapor play a vital role in the by-product generation and catalytic performances.