Two analogous binuclear coordination complexes derived from nitronyl nitroxide radical ligands have been synthesized.Their general formulae are[Mn2(hfac)4(NIT-mo-pmy)2](1)and[Co2(hfac)4(NIT-mo-pmy)2](2),respectively,where hfac=hexafluoroacetylacetone and NIT-mo-pmy=2-(2-methoxy-5'-pyrimidinyl)-4,4,5,5-tetra-methyl-imidazoline-3-oxy-1-oxyl radical.Both complexes crystallize in a triclinic system P1 space group,exhibiting a centrosymmetric rectangle-like array based on dimer coordination units.Variable-temperature magnetic character-izations reveal the presence of antiferromagnetic exchanges between central ions and nitroxide radicals in both four-spin nitroxide radical complexes.The different strengths of both complexes were investigated based on structure-property relationship analysis.The magnetic behaviors of the Mn(Ⅱ)complex have been quantitatively evaluated through an appropriate magnetic model and were compared with the relevant complexes.CCDC:2094992,1;2094993,2.