Treatment of the imines [ArN=CH-CH=NAr] and [ArN=CH-2-py] (Ar = 2,6-Pr i 2 C 6 H 3 ) with AlMe 3 in toluene affords the highly crystalline complexes [AlMe 2 {ArN-CH 2 -C(Me)=NAr}] (1) and [AlMe 2 {ArN-CH(Me)-2-py}] (2); the molecular structures of 1 and 2 show that the aluminiums are bonded to imino-amide and pyridyl-amide ligands respectively arising from methyl group transfer from the aluminium centre to the backbone carbon of the imine ligand.