Metalloenzymes perform some of the most remarkable transformations in nature under ambient conditions in complex cellular milieu. The possibility of leveraging molecular recognition and evolution for non-biological metal catalysts has driven efforts to engineer artificial metalloenzymes (ArMs), hybrid catalysts comprised of synthetic metal cofactors linked to protein scaffolds. In this talk, I will discuss recent efforts from my group to design and evolve ArMs containing dirhodium and metal polypyridine cofactors for selective catalysis.