Two metal-organic coordination polymers of Co II with the molecular formulae [Co(L 1 )(tp)(H 2 O) 2 ] n (1) and [Co(L 2 )(tp)·H 2 O] n (2) [L 1 = 1,4-bis(benzimidazole-1-ylmethyl)-benzene; L 2 = 1,1-(1,4-butanediyl)bis(5,6-dimethylbenzimidazole); tp = terephthalate] were synthesized and characterized by single-crystal X-ray diffraction studies, infrared spectroscopy (IR), thermogravimetric analysis (TGA), X-ray powder diffraction (XRPD), and elemental analysis.Supporting Information (see footnote on the first page of this article): ORTEP plots of the coordination environments; emission spectra; TG curves, and XRPD patterns of compounds 1 and 2.