The single charge transfer through cyanodienes is discussed. The reorganization energies between the neutral molecules and the corresponding monoanions for cyanodienes are larger than those for acenes with D-2h geometry. This result implies that the negatively charged cyanodienes would not be better conductors with slow electron transfer than the negatively charged acenes if we assume that the overlap of the lowest unoccupied molecular orbitals (LUMO) between cyanodienes is not significantly different from that between two neighboring acenes. The structures of the monoanions of cyanodienes are optimized under D-2h geometry, and the vibronic interaction effects in the monoanions of cyanodienes are discussed. The vibration effect on the charge-transfer problem is also discussed. The C-C and C-N stretching A, modes around 1000-1500 cm(-1) are the main modes converting the neutral structures to the monoanions in cyanodienes. This can be confirmed from the calculational results that the C-C and C-N stretching A(g) modes around 1000-1500 cm(-1) strongly couple to the LUMO in cyanodienes. The total electron-phonon coupling constants (l(LUMO)) for the monoanions of cyanodienes are estimated to be larger than those for the monoanions of acenes. The orbital patterns difference between the LUMO localized on carbon atoms located at the edge part of the carbon framework in acenes and the delocalized LUMO in cyanodienes due to electronegativity perturbation is the main reason that the l(LUMO) values for polycyanodienes are much larger than those for polyacenes. The relationships between the electron transfer and the electron-phonon interactions are discussed. The plot of the reorganization energies against the l(LUMO) values is found to be nearly linear. In view of the results, the relationships between the normal and possible superconducting states are briefly discussed.