Abstract. The reaction of Cd(NCS) 2 with 3-hydroxymethylpyridine (3-HMPy) leads to the formation of compounds with the composition Cd(NCS) 2 (3-HMPy) 4 (1-Cd),Cd(NCS) 2 (3-HMPy) 2 (2-Cd)(Cd(NCS) 2 ) 2 -(3-HMPy) 3 (3-Cd), and (Cd(NCS) 2 ) 3 (3-HMPy) 4 (4-Cd). Compound 1-Cd consists of discrete complexes and in 2-Cd the Cd cations are linked into chains by the anionic and the organic co-ligands. In 3-Cd as well as 4-Cd the Cd cations are connected into chains by the thiocyanate anions, which are further linked into layers by the 3-HMPy coligands. In contrast, with Zn only one compound with the composition Zn(NCS) 2 (3-HMPy) 2 ·H 2 O (1-Zn-H 2 O) was characterized by single-