The syntheses of mixed ligand mono metallic [Os(dpop′)(tppz)](PF 6 ) 2 , homo-bimetallic [(dpop′)Os(tppz)Os(dpop′)](PF 6 ) 4 and mixed metal bimetallic [(dpop′)Ru(tppz)Os(dpop′)](PF 6 ) 4 (dpop′=dipyrido(2,3-a:3′,2′-j)phenazine; tppz=2,3,5,6-tetra(2-pyridyl)-pyrazine) complexes is described. NMR spectroscopy was used to confirm pure products were separated from similar species. The 1 H NMR spectrum for the mixed metal Ru/Os bimetallic complex ion reflects additive components of the Ru/Ru and Os/Os bimetallic species. Proton resonances on Ru(II) bonded ligands are upfield from Os(II) bonded ligands. Cyclic voltammetry for the Os/Os and Ru/Os bimetallic complex ions show the reversible tppz 0/−1 reduction at less negative potential than the dpop′ 0/−1 reduction. Additionally, the [(dpop′)Os(tppz)Os(dpop′)] 4+ ion displays reductive coupling of the remote terminal dpop′ ligands that is not observed in the bimetallic Ru/Ru species, indicating larger metal–ligand mixing occurs for Os(II) than Ru(II) complexes. The UV–Vis electronic absorption spectra for all complex ions show intense Os(dπ)→dpop′(π ∗ ) and Os(dπ)→tppz(π ∗ ) MLCT transitions in the visible spectrum with IL transitions in the UV.