Phosphorescent transition metal complexes have been intensively investigated, since these luminophores are distinctively different from fluorescent chromophores in terms of the nature and lifetime scale of photoluminescence (PL). Owing to the inherent differences in the light emission, these metal complexes have been successfully exploited for a variety of optical applications, and some of the studies revealed that phosphorescence is fundamentally important to the experimental results and target performances. Encouragingly, cyclometalated iridium(III) complex is one of the rare entities which shows great potential in various biological and analytical applications, such as luminescent assays, cellular imaging, in vivo imaging and even theranostics. This review article collects the most recent papers on health-related applications by exploiting phosphorescent cyclometalated Ir(III) complexes. At the same time, the structure–property relationships of these Ir(III) complexes will be emphasized throughout the article.