Zr-Ir hydrido complexes with ansa-(cyclopentadienyl)-(amide) as the supporting ligand in the zirconium fragment, e.g., ((LZrR)-Zr-1)(Cp*Ir)(mu-H)(3) [L-1 = Me2Si(eta(5)-C5Me4)((NBu)-Bu-t), R = Cl (5), Ph (7), Me (10), alkyl, and aryl] were designed, synthesized, and isolated as tractable early late heterodinuclear complexes. Despite the presence of the three supporting hydride ligands, Zr-Ir distances in the crystal structures of 5, alkyl, and aryl complexes [2.74-2.76 angstrom] were slightly longer than the sum of the element radii of Zr and Ir [2.719 angstrom]. These hydrocarbyl complexes displayed the thermolytic C H activation of a variety of aromatic compounds and several organometallic compounds. Also, the substrate scope and limitation in the Zr Ir system were studied. The regiochemical outcomes during the C H activation of pyridine derivatives and methoxyarenes suggested the in situ generation of a Lewis acidic active intermediate, i.e., ((LZr)-Zr-1)(Cp*IrH2) (III). The existence of III and relevant a-complex intermediates {(LZr)-Zr-1(eta(2)-R-H)}(Cp*IrH2) (IIR) (R = Me, Ph) in the ligand exchange was demonstrated by the direct isolation of a Et3PO-adduct of III (39b) from 7 and kinetic studies. The structure of the direct Zr-Ir bonds in IIph, IIMe, III, and 39b were probed using computational studies. The unprecedented strong M-M' interactions in the early-late heterobimetallic (ELHB) complexes have been proposed herein.