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Investigation of synthesis and structure of metal complexes is one of the main questions of modern chemistry, where establishment of “structure – property” relationship is a main task. The design of the polydentate ligands (LH2) is crucial to regulate the structure and properties of the metal complexes. In present report the recent results, obtained in our laboratory, on investigation of complexes of Al, Zn, Ti based on polydentate O,N,O-, N,N,N-, O,N,N-, O,N,S- and S,N,S-ligands (synthesis, structure, properties) are presented. Furthermore, 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 obtained are characterized as very active initiators of ring-opening polymerization (ROP) of lactones, where process of polymerization is highly controllable.