We report the synthesis of heterobimetallic Ta-Rh and Ta-Ir complexes bridged by a 2,5-di-tertbutyltantalacyclopentadiene fragment. A mononuclear 2,5-di-tert-butyltantalacyclopentadiene complex 2 was prepared by the reaction of (g 2 -Me 3 SiCCSiMe 3 )TaCl 3 (dme) (1) with excess amounts of 3,3-dimethylbut-1-yne in the presence of AlCl 3 . The tantalacyclopentadiene moiety of complex 2 served as a g 4 -diene unit for coordinating the Rh and Ir centers; treatment of 2 with [M(l-Cl)(cod)] 2 (M = Rh and Ir; cod = cycloocta-1,5-diene) in toluene gave TaRh(l-C 4 H 2 t Bu 2 )Cl 4 (cod) (3) and [TaIr(l-C 4 H 2 t Bu 2 )Cl 4 ] 2 (5), respectively. The X-Ray diffraction study of 3 revealed a dative bond from an electron-rich Rh toward an electron-deficient Ta. Upon dissolving 3 in THF, [(thf)TaRh(l-C 4 H 2 t Bu 2 ) Cl 3 ] 2 (l-Cl) 2 (4) was isolated together with free cycloocta-1,5-diene. When complex 5 was treated with 1,2-bis-(diphenylphosphino)ethane (dppe), a monomeric Ta-Ir complex, TaIr(l-C 4 H 2 t Bu 2 )Cl 4 (dppe) (6), was isolated. Ta-Rh and Ta-Ir heterobimetallic complexes 3 and 6 were reduced by a two-electron process upon reaction with 2,3,5,6tetramethyl-1,4-bis(trimethylsilyl)-1,4-dihydropyrazine (7a: Si-Me 4 -DHP) or 2,5-dimethyl-1,4-bis(trimethylsilyl)-1,4dihydropyrazine (7b: Si-Me 2 -DHP) to afford the corresponding complexes TaM(l-C 4 H 2 t Bu 2 )Cl 2 (L) (8: M = Rh, L = cod; 9: M = Ir, L = dppe), where the metallacycle moiety was assigned to have a tantalacyclopentadiene fragment with a large contribution of a tantalacyclopentatriene canonical form.Bu 2 )TaCl 3 (2), as a unique precursor for reacting with Rh and Ir cyclooctadiene complexes, giving the corresponding Ta-Rh and Ta-Ir heterobimetallic complexes. In these complexes, the diene moiety of the tantalacyclopentadiene served as the