Some new aluminium complexes bearing bidentate monoanionic 2-anilinotroponate ligands have been synthesized and characterized. Reaction of 2-(2,6-diisopropylanilino)tropone or 2-(perfluoroanilino)tropone with AlMe 3 (1 equiv.) gave, by methane elimination, compounds [2-(2,6-diisopropylanilino)tropone]AlMe 2 (1) and [2-(perfluoroanilino)-tropone]AlMe 2 (2), respectively, as yellow solids. Reaction of 1 with 1 equiv. of the ligand furnished, by protodealumination of a second Al−CH 3 bond, the [2-(2,6-diisopropylanilino)tropone] 2 AlMe derivative 3. The structure of 3 has been