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Investigation of metal complexes is one of the main questions of organometallic chemistry, where establishment of “structure – property” relationship is a main task. The design of the polydentate ligands is crucial to regulate the structure and properties of the metal complexes. In present report our results on investigation of the complexes of Al, Zn, Ti, based on polydentate O-, N- and S-ligands are presented. The macromonomer approach, developed in our laboratory, to the modified polymer materials is also presented. It is established that the ligand structure (the size of the chelate ring, nature of the donor atoms, substituents) determines the structure of the complexes formed. All complexes are characterized as active initiators in ring-opening polymerization (ROP) of lactones, whereas process of polymerization is highly controllable.