Highly phosphorescent blue-light-emitting anionic iridium complexes (C4H9)(4)N[lr(2-phenylpyridine)(2)(CN)(2) (1), (C4H9)(4)N[Ir(2-phenyl-4-dimethylaminopyridine)(2)(CN)(2)] (2), (C4H9)(4)N[Ir(2-(2,4-difluorophenyl)-pyridine)2(CN)(2)] (3), (C4H9)(4)N[Ir(2-(2,4-difluorophenyl)-4-dimethylaminopyddine)2(CN)(2)] (4), and (C4H9)4N[lr(2-(3,5-difluorophenyl)-4-dimethylaminopyddine)2(CN)21 (5) were synthesized and characterized using NMR, UV-vis absorption, and emission spectroscopy and electrochemical methods. In these complexes color and quantum yield tuning aspects are demonstrated by modulating the ligands with substituting donor and acceptor groups on both the pyridine and phenyl moieties of 2-phenylpyridine. Complexes 1-5 display intense photoluminescence maxima in the blue region of the visible spectrum and exhibit very high phosphorescence quantum yields, in the range of 50-80%, with excited-state lifetimes of 1-4 mu s in acetonitrile solution at 298 K. DFT and time dependent-DFT calculations were performed on the ground and excited states of the investigated complexes to provide insight into the structural, electronic, and optical properties of these systems.