Bis(tetraethylammonium) dodecamethyl-closo-dodecaborate(2-), [NEt4](2)[closo-B12Me12], [NEt4](2)2, was prepared employing modified Friedel-Crafts reaction conditions from [NE4](2)[closo-B12H12], [NEt4](2)1, trimethylaluminum, and methyl iodide. The [NEt4](2)2 salt provides sufficient solubility in water to allow the synthesis of the important alkali metal salts A(2)2 (A = Li, Na, K, Rb, Cs) using cation-exchange procedures. The solid state structure of colorless [AsPh4](2)2 reveals a nearly perfect icosahedral B-12 cluster with B-B bonds ranging from 1.785(3) to 1.807(3) Angstrom and B-C bonds of 1.597(3)-1.625(3) Angstrom. In contrast, the crystal structure of dark-red [Py2CH2](2) (obtained from [NEt4](2)2 and [Py2CH2]Br-2) contains a distorted icosahedral dianion [B-B = 1.740(13)-1.811-(14) Angstrom, B-C = 1.591(13)-1.704(13) Angstrom]. In the [Py2CH2](2) salt, the dianion 2(2-) and its dipositive dipyridini omethane counterion form a red charge-transfer complex. One-electron oxidation of 2(2-) by ceric(IV) ammonium nitrate affords the blue, air-stable radical [hypercloso-B12Me12](.-), dodecamethyl-hypercloso-dodecaborate(1-), 2(.-), isolated as the PPN salt. X-ray crystallography reveals that the geometries of the B-12 clusters observed in hypercloso-[PPN]2 and closo-[AsPh4](2)2 are identical and essentially undistorted icosahedra. The anion in the [PPN]2 structure contains B-B bonds ranging from 1.784(8) to 1.806(7) Angstrom and a range of B-C bonds from 1.596(7) to 1.616(7) Angstrom.