We report the synthesis of the first early-late heterobimetallic bridging imido complex Cp(2)Zr(mu-N-t-Bu)-IrCp* (1). Complex 1 was synthesized in 65% yield by the sequential addition of n-BuLi and Cp*IrN-t-Bu to Cp(2)ZrCl(2) and was characterized by an X-ray diffraction study. The Ir-Zr bond distance was found to be 2.598(2) Angstrom, and the Ir-N (1.8 87(13) Angstrom) and Zr-N (2.084(13) Angstrom) bond distances are comparable to those observed in analogous homonuclear imido dimers. Imido complex 1 was found to undergo addition of both polar (N-H, O-H, S-H) and nonpolar (H-H, Si-H, C-H) X-H bonds across the Ir-Zr bond. For example, the reaction of imido complex 1 with p-toluidine resulted in the formation of Cp(2)Zr(NHAr)(mu-N-t-Bu) (mu-H)IrCp* (2, 60% yield), the addition of p-cresol gave Cp(2)Zr(OAr)(mu-N-t-Bu)(mu-H) IrCp* (3a, 56% yield), the addition of tert-butyl alcohol led to Cp(2)Zr(O-t-Bu)(mu-N-t-Bu)(mu-H) IrCp* (3b, 74% yield), and the addition of acetone yielded Cp(2)Zr(OC(CH2)CH3)(mu-N-t-Bu)(mu-H)IrCp* (4, 72% yield). Complexes 2 and 3a were characterized by X-ray crystallography. The addition of p-thiocresol yielded two products, 5a and 5b. The major product was found to be spectroscopically similar to the p-toluidine, p-cresol, tert-butyl alcohol, and acetone addition products, suggesting a similar formulation (Cp(2)Zr(SAr)(mu-N-t-Bu)(mu-H)IrCp*). Addition of H2S to 1 resulted in formation of the bridging sulfide complex Cp(2)Zr(mu L-N-t-Bu)(mu-S)IrCp* (6, 45% yield), presumably by a similar X-H addition followed by elimination of H-2. The addition of diethylphosphine and cyclohexylphosphine to imido complex 1 resulted in the unusual insertion of phosphide (PR(2)) into the Ir-N rather than the Ir-Zr bond to give Cp(2)Zr(mu-N(t-Bu)PEt(2))Ir(H)Cp* (8a, 63% yield) and Cp(2)Zr(mu-N(t-Bu)PHCy)Ir(H)Cp* (8b, 50% yield). An X-ray diffraction study was performed on 8a, which revealed that the Ir-Zr bond distance was 2.642(1) Angstrom, comparable to that in imido complex 1.