In the structure of the title compound, [Fe{5-C5(CH3)5}- (NCCH3)(CO)2]BF4, the arrangement of ligands around the Fe atom is in a pseudo-octahedral three-legged piano-stoolfashion in which the pentamethylcyclopentadienyl (Cp*) ligand occupies three apical coordination sites, while the two carbonyl and one acetonitrile ligands form the basal axes of the coordination. The Fe—N bond length is 1.924 (3) A˚ and the Fe—Cp* centroid distance is 1.722 A˚ .