Reaction of {η5 -C5Me5)MoCl 4 with a 10-fold excess of LiBH4 followed by thermolysis with excess BH3·THF in toluene led to the formation of two oxamolybdaborane clusters, (η5-C5Me 5Mo)2B5(μ3OEt)H6R (2, R = H; 3, R = n-BuO). Clusters 2 and 3 have been characterized by 1H, 11B, and 13C NMR spectra and X-ray crystal structure determinations. 2 and 3 are notable examples of oxametallaborane compounds where oxygen is contiguously bound to both the cluster metal (molybdenum) and the boron atom. © 2009 American Chemical Society..