The data set includes the NMR data for the puplication: "The Radical Anion and Dianion of Benzo[3,4]cyclobuta[1,2-b]phenazine".
We present the reduction of two azaarenes, featuring a single cyclobutadiene unit, to their radical anions and dianions. The reduced species were prepared with potassium naphthalenide in the presence of 18-crown-6 in THF. The crystal structures of the reduced representatives were obtained and their optoelectronic properties were evaluated. The charge of these 4n-Hückel systems leads to dianionic 4n+2 π-electron systems with enhanced antiaromaticity according to NICS(1.7)ZZ calculations, which exhibit unusually red-shifted absorption spectra.