In this chapter, we first give a clear definition for single-molecule toroic (SMT) on the basis of the toroidal magnetic moments of ground doublets present in triangular Dy 3 SMMs, which is further exemplified via several typical Dy-based single-molecular magnets (SMMs) showing toroidal magnetic moments. Secondly, we examine the typical polynuclear lanthanide complexes showing SMM behavior, and three main synthetic strategies are given as follows: building block approach, organometallic approach, and multidentate ligand approach. The information extracted from such investigation is expected to enhance our understanding to SMM performances of polynuclear lanthanide complexes and facilitate their future applications.Keywords Single-molecule toroic · Toroidal magnetic moments · Building block · Organometallic approach · Multidentate ligand As mentioned in last two chapters, although the mono-and dinuclear lanthanide complexes have exhibited great achievements in obtaining strongly blocked SMMs due to the strong magnetic anisotropy of lanthanide ions, the limited spin centers in the complexes appear still to prevent the further enhancement of their singlemolecular magnet (SMM) properties due to the limited number of unpaired electrons [1]. Theoretically speaking, the more the spin centers in one metal cluster, the larger spin ground state can be achieved when the ferromagnetic coupling interactions are present in the cluster. Nevertheless, it needs an accurate control for the magnetic anisotropy of each metal center and the magnetic exchange interactions between the metal ions, which seems to be a very challenging task. In particular, it turns to be more difficult for multinuclear lanthanide complexes because the core 4f orbital shielded by the external electrons usually leads to extremely strong magnetic anisotropy of lanthanide ions but poor communication with other metal ions. However, considerable effort of researchers has been devoted to this field, and some groundbreaking results were achieved in this respect. Importantly, the