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Clathrochelate complexes of cobalt are known in the oxidation states I, II, and III. Low‐valent Co(I) complexes are highly reactive compounds, and there is only limited knowledge about their structures in the solid state. Herein, we describe the crystallographic analyses of three low‐valent clathrochelate complexes, along with analyses of the corresponding Co(II) precursors. Two different ligand environments were studied: a) ligands with alkyl substituents, which render the complexes highly reducing, and b) potentially redox non‐innocent ligands. Our analyses show that the ligands have a large effect on the redox potentials, but only a small effect on the geometry and the electronic state of the central Co ion. [ABSTRACT FROM AUTHOR]