Two new green-emitting iridium(III) complexes containing styrene-modified phenylpyridine ligands, namely, Ir(ppy-VB)₂(acac) (Ir-A) and Ir(ppy-VB)₂(Stpip) (Ir-S), where ppy-VB = 2-(4-(((4-vinylbenzyl)oxy)methyl)phenyl)pyridine, acac = acetylacetone, and Stpip = bis(diphenylphorothioyl)amide, have been synthesized and characterized via NMR (¹H and ¹³C) and MS spectroscopy, and the structure of Ir-A has been characterized via single crystal X-ray diffraction. Their photophysical and electrochemical properties and thermal stability were investigated systematically. The results showed that these complexes exhibited green emission, suitable HOMO and LUMO energy levels and good thermal stability.