The reactions of the [Fe(4)S(4)X(4)](2-) cubanes (X = Cl, Br, I), A, with (t)Bu(3)P in CH3CN solution in the presence of NaBPh(4) afford the new, uncharged, mixed-ligand [Fe4S4-((t)Bu(3)P)(3)X] cubanes, B, that contain the [Fe4S4](+) core and show EPR spectra characteristic of a S = 1/2 ground state. In the presence of PhS(-) and PhSSPh, B undergoes ligand exchange and a one e(-) oxidation to give the uncharged, mixed-ligand [Fe4S4((t)Bu(3)P)(2)(SPh)(2)] cubanes, C, that contain the [Fe4S4](2+) core. The solubility of B and C in many common nonpolar solvents makes these clusters ideal for reactivity studies in noncoordinating media.