A study was conducted to develop high external quantum efficiency organic true-blue-light-emitting diodes employing novel design of iridium(III) phosphors. The phosphors were synthesized by a combination of [Ir(tht) 3Cl3] with a stoichiometric amount of bdpH or dfbdpH in decahydronsphthalene, flowed by treatment with fppzH chelate in the presence of Na2CO3. The Ir(III) source and reaction solvent was intended to suppress the metal-hydride formation that was encountered in protic solvents, such as methoxyethanol and its analogues. Single-crystal X-ray diffraction of phosphors [Ir(fppz)2(bdp)] was carried out to determine its molecular structure. Significant information was also provided about the quantum efficiency of the OLEDs through a time-dependent density function theory (TD-DFT) approach.