Of the three known low-nuclearity iron-sulfur clusters in metallobiomolecules with the core units Fe2S2 Fe4S4, and Fe3S4, the last has not been obtained in stable form outside a protein environment. We describe a direct route to such clusters in the [Fe3S4](0) oxidation state, and demonstrate an effective stereochemical and electronic structural congruence with the native cluster. The synthesis is based on iron-site-differentiated clusters. Reaction of [Fe4S4(LS(3))(SEt)](2-) with (Et(3)NH)(OTf) affords [Fe4S4(LS(3))(OTf)(2-), whose unique site is activated toward terminal ligand substitution. Treatment with 1 equiv of (Et(4)N)(2)(Meida) affords [Fe4S4(LS(3))(Meida)](3-), which is readily converted to [Fe3S4(LS(3))](3-) with 1-2 equiv of additional reactant. The trinuclear cluster is formed by abstraction of Fe2+ from a precursor cubane-type [Fe4S4](2+) core and complexation as [Fe(Meida)(2)](2-). An analogous procedure starting with [Fe4Se4(LS(3))(SEt)](2-) yields [Fe3Se4(LS(3))](3-). The compound (Et(4)N)(3)[Fe3S4(LS(3))]. MeCN crystallizes in orthorhombic space group P2(1)2(1)2(1) with no imposed symmetry. An X-ray structure solution demonstrates the presence of the desired cuboidal [Fe-3(mu(3)-S)(mu(2)-S)(3)](0) core in a complex of absolute configuration Delta.