The dissociative and abstractive chemisorption dynamics of NO on Al(111) were studied. A higher sticking probability for the N end-on of NO onto Al(111) was measured. In contrast, Auger electron experiments reveal stepped surfaces to be oxygen rich at low coverage after exposure to NO. Density functional theory calculations show (i) a few angstroms from the surface, an N end-on first collision geometry results in electronic structures consistent with charge transfer; (ii) there is stabilization on the surface for N end-on or side-on orientations; (iii) dissociation is enhanced by a partial or full flip of the molecule.