Three novel iron(III) complexes of 2-benzoylpyridine N(4), N(4)-(butyl-1,4-diyl) thiosemicarbazone (HBpypTsc), [Fe(BpypTsc) 2 ]ClO 4 (1), [Fe(BpypTsc) 2 ]NO 3 (2) and [Fe(BpypTsc) 2 ]FeCl 4 (3) were synthesized and physico-chemically characterized by means of partial elemental analyses, magnetic measurements (polycrystalline state), UV-Vis and IR spectroscopies. The spin Hamiltonian parameters, isomer shifts and quadrupolar splitting values of the complexes were assigned by variable temperature EPR and Mossbauer spectra. The presence of a spin-paired iron(III) cation with d x z 2 d y z 2 d x y 1 ground state is revealed by the simulated EPR spectral data. The structures of the free ligand HBpypTsc and one of the complexes [Fe(BpypTsc) 2 ]FeCl 4 (3) were solved by single crystal X-ray diffraction which authenticated a FeN 4 S 2 octahedral coordination in the complex, as envisaged from the spectral data. All complexes except [Fe(BpypTsc) 2 ]FeCl 4 (3) were found to be low-spin S=1/2 ( 2 T 2 g ), whereas 3 was found to have both low-spin ( 2 T 2 g ) and high-spin ( 6 A 1 ) centres.