Two new cationic iridium complexes, [Ir(ppy)2(phpzpy)]PF6 (complex 1) and [Ir(dfppy)2(phpzpy)]PF6 (complex 2), bearing a 2-(3-phenyl-1H-pyrazol-1-yl)pyridine (phpzpy) ancillary ligand and either 2-phenylpyridine (Hppy) or 2-(2,4-difluorophenyl)pyridine (Hdfppy) cyclometalating ligands, were synthesized and fully characterized. The photophysical and electrochemical properties of these complexes were investigated by means of UV-visible spectroscopy, emission spectroscopy, and cyclic voltammetry. Density functional theory (DFT) and time dependent DFT (TD-DFT) calculations were performed to simulate and study the photophysical and electrochemical properties of both complexes. Light-emitting electrochemical cells (LECs) were fabricated by incorporating complexes 1 and 2, which respectively exhibit blue-green (488 and 516 nm) and blue (463 and 491 nm) emission colors, achieved through the meticulous design of the ancillary ligand. The luminance and current efficiency measurements recorded for the LEC based on complex 1 were 1246 cd m(-2) and 0.46 cd A(-1), respectively, and were higher than those measured for complex 2 because of the superior balanced carrier injection and recombination properties of the former.