4CH 3 OH (2) coordination complexes have been prepared by the reaction of the tetradentate H 2 pmide ligand and Cu(NO 3 ) 2 ·3H 2 O or Co(CH 3 CO 2 ) 2 ·4H 2 O/NaNCS in organic solvent (H 2 pmide = N-(2-pyridylmethyl)iminodiethanol). In 1, one copper(II) ion is bonded with a H 2 pmide, and the other is coordinated with a mono-deprotonated Hpmide − . The copper(II) ions are linked through an ethoxo group of the Hpmide − ligand and two oxygen atoms of a nitrate ion, resulting in an asymmetric dinuclear structure. In 2, two terminal cobalt(III) units are coordinated with pmide 2− , NCS − , and CH 3 CO 2 − . The terminal units are each connected to a central cobalt(II) cation through the two oxygen atoms of pmide 2− and one bridged acetate ion, giving rise to a mixed-valence trinuclear cobalt complex formulated as Co III -Co II -Co III . Complex 1 shows a strong antiferromagnetic interaction through the ethoxo and nitrato groups between the copper(II) ions [g = 2.070, J = -88.1 cm −1 (-61.2 K)]. However, complex 2 behaves as a paramagnetic cobalt(II) monomer, due to the diamagnetic cobalt(III) ions in the terminal units [g = 2.526, |D| = 51.8 cm −1 (36.0 K)]. † CCDC 1402754 and 1402755. For crystallographic data in CIF or other electronic format see