| Summary: | Two cadmium(II) coordination polymers, with thiocyanate and pyridine-based ligands e.g., 3-acetamidopyridine (3-Acpy) and niazid (nicotinic acid hydrazide, nia), namely one-dimensional {[Cd(SCN)<sub>2</sub>(3-Acpy)]}<i><sub>n</sub></i> (<b>1</b>) and two-dimensional {[Cd(SCN)<sub>2</sub>(nia)]}<i><sub>n</sub></i> (<b>2</b>), are prepared in the mixture of water and ethanol. The adjacent cadmium(II) ions in <b>1</b> are bridged by two <i>N</i>,<i>S</i>-thiocyanate ions and an <i>N</i>,<i>O</i>-bridging 3-Acpy molecule, forming infinite one-dimensional polymeric chains, which are assembled by the intermolecular N–H∙∙∙S hydrogen bonds in one direction and by the intermolecular S∙∙∙S chalcogen bonds in another direction. Within the coordination network of <b>2</b>, the adjacent cadmium(II) ions are bridged by <i>N</i>,<i>S</i>-thiocyanate ions in one direction and by <i>N</i>,<i>O</i>,<i>N’</i>-chelating and bridging nia molecules in another direction. The coordination networks of <b>2</b> are assembled by the intermolecular N–H∙∙∙S and N–H∙∙∙N hydrogen bonds and S∙∙∙S chalcogen bonds. Being the only supramolecular interactions responsible for assembling the polymer chains of <b>1</b> in the particular direction, the chalcogen S∙∙∙S bonds are more significant in the structure of <b>1</b>, whilst the chalcogen S∙∙∙S bonds which act in cooperation with the N–H∙∙∙S and N–H∙∙∙N hydrogen bonds are of less significance in the structure of <b>2</b>.
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