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Treatment of a dirhodium analogue of pentaborane(9), [(Cp*Rh)2B3H7] (nido‐1; Cp* = η5‐C5Me5), with [Fe2(CO)9] at room temperature led to the formation of [(Cp*Rh)2Fe(CO)3(µ‐CO)B3H2Cl] (2) and the metal‐rich metallaborane [(Cp*Rh)2Fe(CO)3Fe(CO)2(µ‐CO)2B2H2] (3). When the same reaction was carried out at moderate temperature, two metal‐rich metallaboranes, [(Cp*Rh)3Fe(CO)2(µ3‐CO)2B2HX] 4 (X = H) and 5 (X = Cl), and a heterometallic µ9‐boride cluster, [(Cp*Rh)3(RhCO)3Fe(CO)3(µ‐CO)3B3H2] (6), were obtained. Compounds 4 and 5 can be viewed as cubane clusters with 62 cluster valence electrons (cves) and five metal–metal bonds. In another reaction, the treatment of nido‐1 with [Mn2(CO)10] yielded the heterometallic µ9‐boride cluster [(Cp*Rh)3Rh(CO)2{Mn(CO)3}2B4H3] (7). The cluster cores of both 6 and 7 are comprised of tricapped trigonal prisms containing a µ9‐B atom bonded to seven/six metals and two/three boron atoms, respectively. All the new compounds have been characterized by mass spectrometry, IR, 1H, 11B{1H}, and 13C{1H} NMR spectroscopy, and X‐ray crystallographic analysis. [ABSTRACT FROM AUTHOR]