The aluminium complexes {[k 2 -N,O-(t-BuNCOPh)]AlMe 2 } 2 (2), [k 2 -N,O-(t-BuNCOPh)] 2 AlMe (3), and [k 2 -N,O-(t-BuNCOPh)] 3 Al (4) were prepared through the protonolysis reaction between trimethylaluminium and one, two, or three equivalents, respectively, of N-tert-butylbenzamide. Complex 2 was also prepared via a salt metathesis reaction between K(t-BuNCOPh) and dimethylaluminium chloride. Complexes 2-4 were characterized using 1 H and 13 C NMR spectroscopy. Single-crystal X-ray diffraction analysis of the complexes corroborated ligand : metal stoichiometries and revealed that all the amidate ligands coordinate to the aluminium ion in a k 2 fashion. The Al-amidate complexes 2-4 were viable catalyst precursors for the Meerwein-Ponndorf-Verley-Oppenauer reduction-oxidation manifold, successfully interconverting several classes of carbonyl and alcohol substrates.The 1 : 1 reaction between trimethylaluminium and various simple amides has been previously reported by the Lin group [31,32] who showed that the bonding mode of the ligand and solid-state structure of the Al-amidate complexes were dependent on the substitution pattern of the amide precursor.