The reaction of [Cp*MoCl 4] with an excess of LiBH 4, followed by thermolysis with tellurium powder in toluene, afforded a tricapped cubane cluster, [(Cp*Mo) 4B 4H 4(μ 4-BH) 3] (1), which represents an unprecedented metal-rich metallaborane cluster with a cubane core containing 58 cluster valence electrons (cve) and three metal-metal bonds. © 2011 American Chemical Society.