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Fused‐pentagons results in an increase of local steric strain according to the isolated pentagon rule (IPR), and for all reported non‐IPR clusterfullerenes multiple (two or three) metals are required to stabilize the strained fused‐pentagons, making it difficult to access the single‐atom properties. Herein, we report the syntheses and isolations of novel non‐IPR mononuclear clusterfullerenes MNC@C 76  (M=Tb, Y), in which one pair of strained fused‐pentagon is stabilized by a mononuclear cluster. The molecular structures of MNC@C 76  (M=Tb, Y) were determined unambiguously by single‐crystal X‐ray diffraction, featuring a non‐IPR  C  2 v  (19138)‐C 76  cage entrapping a nearly linear MNC cluster, which is remarkably different from the triangular MNC cluster within the reported analogous clusterfullerenes based on IPR‐obeying C 82  cages. The TbNC@C 76  molecule is found to be a field‐induced single‐molecule magnet (SMM).

Mononuclear Clusterfullerene Single‐Molecule Magnet Containing Strained Fused‐Pentagons Stabilized by a Nearly Linear Metal Cyanide Cluster