The adsorption and dissociation of three carbonyl compounds, formaldehyde, acetaldehyde, and acetone, on the magnesium oxide nanosurface, consisting of four stacked (MgO)(3) hexagons, is investigated by first principles density functional theory (DFT). In the case of formaldehyde, strongly chemisorbed species, with carboxylate-like structures, are initially formed. These may subsequently undergo heterolytic cleavage of an aldehyde CH bond to form formate ions involving a surface oxide ion and a hydride ion adsorbed over the magnesium dication [(MgH+)(HCOO-)]. For acetaldehyde, besides this reaction leading to the formation of acetate, the methyl hydrogen of the adsorbed species also tends to attach itself to a surface oxide ion, yielding surface hydroxyl ions and adsorbed [CH2C(H)OMg](+). These results are in accord with our previous experimental and theoretical results. In particular, the shift of the aldehyde CH vibration band to higher frequency and the appearance of OH bands in the infrared spectrum are clearly accounted for. For acetone, the mechanism is found to be similar, i.e., a methyl hydrogen shift to yield surface enolate. Again, this is in agreement with experimental studies.