We report the synthesis and characterisation of a family of three CoII4 and two CoII3 complexes from a symmetrical diazine ligand, H2hyda = N,N-bis(3-methoxy salicylidene)hydrazine. The metallic skeletons of all complexes reveal a nearly linear arrangement of CoII centers. The present results highlight the profound influence of anions on the structural outcome of a complex. Furthermore, distortion imposed by the twisted nature of the diazine-based ligand depends on the use of associated anions which results in triple helical CoII4 and double helical CoII3 entities. The CoII ions in complexes 1–3 are antiferromagnetically coupled leading to an S = 0 ground state. In contrast, complexes 4 and 5 exhibit a magnetic ground state, but exhibit different behaviours at low temperatures due to differences in crystal packing and hence intermolecular interactions.
