The title compound 1 was prepared by a one pot double-deprotonation, migration, and oxidation sequence starting with (mu,eta(6):eta(6)-2,2'-biindenyl)Mo-2(CO)(6) (2). An X-ray structure was determined, and the relevant structural features are compared with analogous fulvalene and dibenzo[a,d]fulvalene complexes. The reactions of 1 with 4-octyne and P(CH3)(3) are described. Compound 1 is a more effective catalyst in the Kharasch reaction than other bimetallic molybdenum complexes.