High-frequency/high-field electron paramagnetic resonance studies on two homonuclear 12-MC-4 metallacrown complexes Cu 4 Cu and Co 4 Co are presented. For Cu 4 Cu, our data imply axial-type g-anisotropy with g x = 2.03 ± 0.01, g y = 2.04 ± 0.01, and g z = 2.23 ± 0.01, yielding g = 2.10 ± 0.02. No significant zero field splitting (ZFS) of the ground state mode is observed. In Co 4 Co, we find a m S = ±3/2 ground state with g = 2.66. The data suggest large anisotropy D of negative sign.