Dinuclear Fe and Ni complexes, [(phenO)Fe(N )] (NO ) (1) and [(phenOH)Ni(N ) ] (2), were prepared by treating Fe(NO ) ⋅9 H O and Ni(NO ) ⋅6 H O in methanol, respectively, with phenOH (=N-(2-pyridylmethyl)-N'-(2-hydroxyethyl)ethylenediamine) and NaN ; both 1 and 2 were characterized by elemental analysis, IR spectroscopy, X-ray diffraction, and magnetic susceptibility measurements. Two ethoxo-bridged Fe and two azido-bridged Ni were observed in 1 and 2, respectively; corresponding antiferromagnetic interaction via the bridged ethoxo groups and strong ferromagnetic coupling via the bridged end-on azido ligands within the dimeric unit were observed. Complex 1 did not exhibit any catalytic activity, while 2 exhibited excellent catalytic activities for the epoxidation of aliphatic, aromatic, and terminal olefins.