The optimized geometries, electron affinities, and vibrational frequencies of perfluoro polycyclic aromatic hydrocarbon radicals, namely, C6F5, C10F9, and C14F9, have been studied using four density functional theory methods in conjunction with augmented double-xi plus polarization (DZP+) basis sets. Three measures of neutral/anion energy differences reported in this work are the adiabatic electron affinity, the vertical electron affinity, and the vertical detachment energy. The vibrational frequencies of these radicals are also examined. The reliable predicted adiabatic electron affinities [DZP+ B3LYP (Becke's three-parameter hybrid exchange functional with the Lee, Yang, and Parr correlation functional)] are 3.24 eV (for C6F5), 3.04 eV (alpha) and 3.34 eV (beta) for the two isomers of C10F7, and 3.14 eV (alpha), 3.46 eV (beta), and 2.83 eV (gamma) for the three isomers of C14F9.