Three lanthanide-nitronyl nitroxide radical compounds [Ln(hfac)(3)(NIT-Ph-4-Br)(2)] (Ln=Gd(1), Tb(2), Dy (3), hfac=hexafluoroacetylacetonate, NIT-Ph-4-Br=2-(4'-bromide)-4,4,5,5-tetramethyl-imidazoline-1-oxy1-3-oxide) have been successfully prepared and characterized by single crystal X-ray diffraction, IR spectroscopy and elemental analyses. Single crystal X-ray crystallographic analyses reveal that all these three compounds are isostructural and crystallize in the P2(1)/c space group, which are composed of one Ln (hfac)3 unit and two NIT-Ph-4-Br radicals. Magnetic studies reveal that ferromagnetic interactions and antiferromagnetic interactions coexist in Gd complex and there are very weak ferromagnetic interactions between LnOTO ions and the coordinated nitronyl nitroxide in Tb complex and Dy complex. CCDC: 1496095, 1; 1496096, 2; 1496097, 3.