Single-electron oxidation of neutral boryl-linked tetraaminoethylene derivatives 4 led to the formation of radical cations 4˙⁺, which have been isolated and fully characterized. X-ray diffraction analysis, EPR spectroscopy, and computational studies revealed that the unpaired electron is delocalized over the B₂N₄C₂ skeleton and the spin density mainly resides on the carbon and boron atoms.