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This paper describes a new mutual transformation mode occurred between two aluminium complexes, L1(AlMe2)2·AlMe3 and (L1AlMe)2, which were generated upon different solvents and bearing the oxazoline‐amido‐phenolate ligand. Density functional theory (DFT) studies support plausible mechanisms. Their catalytic studies were investigated towards ring opening polymerization of ε‐caprolactone and l‐lactide...