The cyano-bridged molecular square Ni(iprtacn)] 2 [Fe(phen) 2 (CN) 2 ] 2 (PF 6 ) 4 ·6CH 3 CN (1) (iprtacn = 1,4,7-triisopropyl-1,4,7-triazacyclononane, phen = 1, 10-phenanthroline) was prepared and its crystal structure, magnetic properties, and binding with DNA were characterized. The four metal ions Ni II Fe II Ni II Fe II of the complex 1 are almost coplanar. Magnetic susceptibilities measured