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Self-assemblies of two unsymmetrical tridentate N 2 O/N 2 S donor Schiff base ligands, that is, 2-((2-(dimethylamino-)ethylimino)methyl)phenol (HL 1 ) and methyl-2-pyridylmethylidenehy-drazinecarbodithioate (HL 2 ), with different cadmium salts have led to 11 anion-controlled complexes, namely, [Cd(, and [CdL 2 (SCN) 2 ] n (10), respectively. Eleven compounds were characterized by elemental analyses, IR spectra, MS and thermogravimetric analyses, of which 10 structures 2,