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Macrocycle ligands have three or more donor sites. Selective replacement of skeleton carbon atoms by heteroatoms and vacancies in C₆₀ could lead to various macrocycle ligands with a cage‐shaped backbone. Theoretical calculations indicate that such C₆₀‐based macrocycle ligands are as stable as C₆₀ thermodynamically according to their similar HOMO–LUMO gaps. The synthesis of these ligands is a challenging task. Nevertheless important progresses have been reported. This concept article focuses on the structures of possible C₆₀‐based macrocycle ligands and related synthetic results.