Based on the dithiolene chemistry, a systematic research of the transition metal coordination complexes [RBzPyR][M(nmt)2] (mnt =maleonitriledithiolate) have been established, which showed novel phase-and magnetic transitions.By switching the substituting groups on the cationic pyridinium components and relevant crystal engineering, tunable crystal architectures and sequentially inducible magnetic properties of these complexes were explored in our lab.In the meantime, the inclusion complexes of above-mentioned metal complexes anions with natural or semi-synthetic cyclodextrins were studied as well.