The crystal structure of the title compound, [Fe(CS2NBu2)3], C6H6, has been determined at 295 K from diffractometer data and refined by least squares to a residual of 0.071 for 3077 ‘observed’ reflections. Crystals are orthorhombic, Pncn, a = 23.660(9), b = 17.331(7), c = 10.349(9) Å. Unlike the unsolvated derivative, the present compound has a magnetic moment of 3.6 B.M. at 295 K. Its molecular symmetry is 2, (FeS) being 2.34, Å. The role of the benzene solvent, at a lattice site, is not indicative of any strong intermolecular interaction.