AbstractRemoval of two electrons from 1,8‐bis(4‐methylphenylthio)‐9‐(2, 6‐dimethoxyphenyl‐1‐13C)‐10‐phenylanthracene(2)provides stable dication1. Isotopic enrichment (85%) of13C at the labeled site of the aromatic carbon, between the two sulfurs, makes possible the observation of spin‐spin coupling constants between this13C‐carbon and the directly bonded equatorial ligand carbons. The magnitudes of these coupling constants (two1JC1′C2′= 61.9 Hz and one1JC1′C9= 56.3 Hz) suggest that this carbon is sp2hybridized, with the postulated trigonal bipyramidal (TBP) geometry about this carbon center. The13C NMR chemical shifts for the 10‐C‐5 carbon (δ109.3) and for other carbons provide strong evidence against alternative structures for this dication. The data are consistent with the 10‐C‐5 species, with apical sulfonium ligands and equatorial carbons of