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Two novel heteroleptic iridium complexes containing 4-phenylquinazoline (pqz) as a cyclometalating ligand, namely Ir1 and Ir2, are designed and synthesized. Methoxy groups are incorporated into the 6- and 7-sites of pqz rings to tune the physical properties and the emission performance of the complexes. The introduction of methoxy groups in Ir1 and Ir2 causes a slight blue shift by 3–5 nm relative to the reference complex Ir(pqz)2(acac) (630 nm), and moderate photoluminescence quantum yields of 0.35 and 0.38 and short lifetimes of 0.79 and 0.64 μs, respectively, are obtained. Ir1 and Ir2 are used as doped emitters to fabricate phosphorescence organic light-emitting diodes and pure red electroluminescence (EL) is achieved. In comparison with the reference complex Ir(pqz)2(acac), dramatically improved EL performance with color purity and efficiencies are realized for both Ir1 and Ir2. In particular, the Ir2 device exhibits a maximum external quantum efficiency of 26.22% with Commission Internationale de l'Eclairage (CIE) coordinates of (0.65, 0.34), which is close to the best efficiencies reported for other pqz based red iridium phosphors but advantageous in terms of a simple device structure with a single emitting layer. [ABSTRACT FROM AUTHOR]