The coordination chemistry of the unusual metallo‐ligand Cs⊂[CpCo(CN)3]4[Cp*Ru]3 (Cs⊂Co4Ru3) is described with attention to the behavior of the ligand itself, its binding to Lewis‐acidic metal cations, and its ability to stabilize catalytically relevant Ru–PPh3 fragments. A series of tests demonstrate that the “rim” [CpCo(CN)3]– groups in Cs⊂Co4Ru3 are exchangeable. Upon treatment with [(MeC5H4)Co(CN)3]– (Co′) Cs⊂Co4Ru3 undergoes vertex exchange to give Cs⊂Co4–xCo′xRu3. Similarly the cage is degraded by CO. Most convincing, Cs⊂Co4Ru3 reacts with PhNH3OTf to precipitate the polymer PhNH3CpCo(CN)3 and form the molecular box [Cs⊂Co4Ru4]+. Treatment of Cs⊂Co4Ru3 with [M(NCMe)x]PF6 (M = Cu, Ag) gave the Lewis acidic cages {Cs⊂[CpCo(CN)3]4[Cp*Ru]3M(NCMe)}PF6, which reacted with tertiary phosphane ligands to give adducts [Cs⊂Co4Ru3M(PPh3)]PF6. Lewis acidic octahedral vertices were installed using Fe, Ni, and Ru reagents. The boxes [Cs⊂Co4Ru3M(NCMe)3]2+ (M = Ni, Fe) formed readily from the reaction Cs⊂Co4Ru3 with [Ni(NCMe)6](BF4)2 and [Fe(NCMe)6](PF6)2. Displacement of the MeCN ligands gives [Cs⊂Co4Ru3Ni(9‐ane‐S3)](BF4)2. A series of boxes were prepared by the reaction of Cs⊂Co4Ru3 and RuCl2(PPh3)3, RuHCl(PPh3)3, and [(C6H6)Ru(NCMe)3](PF6)2. The derivative of the hydride, [Cs⊂Co4Ru3Ru(NCMe)(PPh3)2](PF6)2, was characterized crystallographically.(© Wiley‐VCH Verlag GmbH & Co. KGaA, 69451 Weinheim, Germany, 2007)