Group 9 metal complexes based on iridium and rhodium have recently arisen as fascinating potential alternatives to existing platinum and ruthenium metallodrugs. While long regarded as chemically inert, studies over the past few years have demonstrated that the reactivity and biological activity of iridium and rhodium complexes may be unlocked by a suitable choice of auxiliary ligands. In addition, group 9 metal centers have received increased popularity for the construction of kinetically inert organometallic scaffolds as target-selective protein or enzyme inhibitors. In this review, we summarize the recent strategies that have been utilized for the design and development of bioactive iridium and rhodium complexes.