The synthesis, structural characterization and magnetic study of novel Co II /4f and Co II /Y III clusters are described. In particular, the initial employment of di-2-pyridyl ketone, (py) 2 CO, in mixed metal Co/4f chemistry, provided access to four triangular clusters,is the monoanion of the hemiketal form of (py) 2 CO. Clusters 1-4 are the first reported Co/4f (1-3) and Co/Y (4) species bearing (py) 2 CO or its derivatives, despite the fact that over 200 metal clusters bearing this ligand have been reported so far. Variable-temperature, solid-state dc and ac magnetic susceptibility studies were carried out on 1-4 and revealed the presence of weak ferromagnetic exchange interactions between the metal ions (J Co-Co = +1.3 and +0.40 cm −1 in 1 and 4, respectively; J Co-Gd = +0.09 cm −1 in 1). The ac susceptibility studies on 2 revealed nonzero, weak out-of-phase (χ" M ) signals below~5 K.