Reactions of cadmium(II) salts with 3-amino-5-methylthio-1H-1,2,4-triazole (Hamstz) afforded two cadmium(II) coordination polymers, [Cd2(amstz)2Cl2]n(1) and [Cd2(amstz)2(NO3)2]n(2). Compounds1and2feature 2-D layered structures based on the dinuclear [Cd2(amstz)2] subunits. The cadmium coordination polyhedra are tetrahedral and tetragonal pyramidal in1and2, respectively, due to the presence of different coordinated anions, Cl−and NO3−. Compounds1and2exhibit photoluminescence emission with maxima at 620 and 621 nm upon excitation at 470 and 472 nm, respectively, which can be attributed to the ligand-to-metal charge transfer emssion. [ABSTRACT FROM AUTHOR]