Three DyIII SMMs were obtained with Schiff-base ligands containing nitro-groups. The triangular complex supported by the cis–trans form of the hnc3− ligand displayed the first air-stable triangular complex with a N–N pathway.

Using the Schiff‐base ligand 1,5‐bis(salicylidene)carbohydrazide (H3bsc) a unique dinuclear dysprosium(III) compound, [Dy2(µ‐OH)(bsc) (NO3)2(DMF)3(H2O)]·THF·2DMF (1·THF·2DMF), has been synthesized. The structural and magnetic properties are fully studied and single‐molecule magnetic behavior with an energy barrier (Ueff = 123 K) has been observed.