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The crystal and molecular structures of the one-dimensional coordination polymer [Zn(S 2 COEt) 2 ( 4 LH 2 )] n  ( 1 ) and binuclear [Zn(S 2 COCy) 2 ] 2 ( 4 LH 2 ) ( 2 ) are described, where  4 LH 2  is N,N′-bis(pyridin-4-ylmethyl)ethanediamide. In  1 , the Zn(S 2 COEt) 2  entities are linked by bidentate bridging  4 LH 2  ligands through the pyridyl-N atoms to generate a twisted supramolecular chain. As a result of monodentate xanthate ligands, the N 2 S 4  donor set defines a distorted tetrahedral coordination geometry and, crucially, allows the participation of the non-coordinating sulfur atoms in supramolecular association. Thus, in the crystal amide-N–H···O(amide) and amide-N–H···S(thione) hydrogen bonds link chains into a three-dimensional architecture. The substitution of the ethyl group in the xanthate ligand with a cyclohexyl group results in very different structural outcomes. In  2 , a binuclear molecule is observed with the coordination geometry for zinc being defined by chelating xanthate ligands and a pyridyl-N atom with the NS 4  donor set defining a highly distorted geometry. In the molecular packing, amide-N–H···S(thione) hydrogen bonds stabilise a supramolecular chain along the a-axis and these are connected into a three-dimensional arrangement by methylene-C–H···O and methylene-C–H···π(pyridyl) interactions. The relative importance of the specified intermolecular interactions and weaker, contributing contacts has been revealed by an analysis of the calculated Hirshfeld surfaces of  1  and  2 .

Steric control of supramolecular association in structures of Zn(S 2 COR) 2 with N , N ′-bis(pyridin-4-ylmethyl)oxalamide