This work illustrates the promise of simple iridium(III) (NHC) complexes as photocatalysts in a broad range of transformations. Both isomers of Ir(pmi)3 were shown to be attractive alternatives to fac-Ir(ppy)3, broadly achieving better yields across a range of energy transfer, photoredox, and metallaphotoredox reactions owing to their higher ET (by ~0.9 eV) more negative E*ox (by ~ 1 V) and superior photostability. Additionally, for the 1,3-sigmatropic shift of s-verbenone, fac-Ir(ppy)3 was unable to sensitize the substrate, while using fac-and mer-Ir(pmi)3 resulted in comparable yields of 62 and 64%, respectively. This work highlights the value and utility of accessing PCs that are simultaneously strongly photoreducing and can sensitize substrates with very high ET. When compared to other strongly photoreducing and high triplet energy Ir(III) photocatalysts, Ir(pmi)3 is particularly attractive for its relatively simple synthesis, high photostability and versatility in photocatalyzing different reaction classes. To the best of our knowledge this study is the first investigation into the use of homoleptic Ir(III) NHC complexes as photoredox and metallaphotoredox catalysts. It is also the first investigation into the stability of these complexes for photocatalysis, in which we found, in particular, fac-Ir(pmi)3 to be an exceptionally stable photocatalyst, and into the difference in reactivity between facial isomers of any transition metal PC. We hope that this report inspires further investigation into the use of iridium(III)