Beyond that quantum-chemical characterization the [Cp* 2 Co] + 2 [TCNQ•4 B(C 6 F 5 ) 3 ] 2ꟷ had sufficient solubility in CD 2 Cl 2 to allow its characterization via multinuclear NMR spectroscopy. Two signals in the 1 H-NMR can be assigned to the TCNQ protons (δ = 6.82 ppm) as well as the methyl protons of decamethylcobaltocenium (δ = 1.65 ppm). In the B NMR spectrum a broad signal at δ = -11.5 ppm is assigned to the tetracoordinate boron atoms in [TCNQ•4 B(C 6 F 5 ) 3 ] 2ꟷ which is also in agreement with other nitrogen-containing adducts. For example, [CH 3 CN•B(C 6 F 5 ) 3 ] has a 11 B NMR shift of -10.3 ppm (in C 6 D 6 ). In comparison the 11 B NMR shift of uncoordinated B(C 6 F 5 ) 3 is observed at +59.2 ppm. In the In the first two cases EPR spectra showed the presence of two radical species each: the corresponding, well-known radical cations as well as the desired radical anion. In the last case only the spectrum of [TCNQ•4 B(C 6 F 5 ) 3 ] ꟷ was observed, since ferrocenium is not EPR-active at room temperature. The EPR spectrum of the radical anion [TCNQ•4 B(C 6 F 5 ) 3 ] ꟷ consists of one broad, isotropic signal at g iso ≈2.002 which confirms the strong delocalization of the unpaired electron. Hyperfine splitting was not observed due the large number of spincarrying nuclei as well as the presence of isotopomers (natural abundance of 10 B = 20%, I=3, and B with 80% abundance and I=3/2). In summary, we report a potent oxidation system from commercially available chemicals that works in non-coordinating organic solvents and is easy to use. The combination of TCNQ with four equivalents of B(C 6 F 5 ) 3 is able to quantitatively oxidize substrates up to an oxidation potential of E ≈ +0.9 V and generates large, previously unknown weakly-coordinating anions that are redox-active. The resulting [TCNQ•4 B(C 6 F 5 ) 3 ] ꟷ monoanion has still enough oxidation power to oxidize ferrocene to ferrocenium. We are optimistic that similar systems (using cyanocarbons in combination with Lewis acids) could not only be used in molecular chemistry, but will also of interest for the doping of organic polymers.