“…Generally speaking, high magnetic density, which guarantees the large metal/ligand mass ratio, is favorable to enhance the MCE. In this sense, a successful approach that has been proposed to obtain the larger MCE is to construct Gd III ions with light and multidentate organic or inorganic ligands. − Accordingly, a number of Gd-clusters and coordination polymers with various structures have been constructed and investigated, and the maximum value of −Δ S m has been continuously exceeded. − Nonanuclear Ln-clusters, especially those with a sandglass topology, were attractively synthesized, but the MCE of Gd complexes was usually neglected. − Admittedly, it remains a challenge for researchers to availably design and synthesize the limited high nuclearity Gd-clusters that afford interesting structural features and high MCE because of several challenges in synthesizing this type of clusters, such as the coordination modes of the ligands, anion templates, the ratio of raw materials, the pH value, solvents, as well as the temperature. Furthermore, apart from high magnetic density, the large MCE of Gd-clusters is also dependent upon weak magnetic couplings between the metal ions.…”