The aim of this perspective is to summarise the use of the reported 3d-4f Coordination Clusters (CCs) in catalytic reactions and to demonstrate the potential of this emerging field. The pioneering work of Shibasaki, Matsunaga and others, demonstrated the use of 3d-4f in situ systems to catalyse asymmetric organic transformations. Our recent studies show that well characterised 3d-4f CCs catalyse numerous organic transformations and useful mechanistic aspects of their catalysis can be obtained. Furthermore, we have shown that by manipulation of the metal ion coordination environment; the nature of the 3d and lanthanide ions and the organic periphery of the ligand can all improve the efficacy of a 3d-4f CC catalyst. All in situ formed and well characterized 3d-4f CCs involved in catalysis are discussed.