Resonance Raman spectra and vibrational analysis based on density functional theory calculation of formylferrocene thiosemicarbazone (TFF) are presented for the first time, together with resonance Raman spectra of ferrocene (FeCp). Raman excitation profiles for several modes of both molecules in the solid state exhibit a minimum, characteristic of antiresonance effect, in the region of d-d transition of the ferrocenyl moiety. The excitation profiles of FeCp obtained from solution also present a deenhancement in the d-d transition region. These behaviors are in contrast with previous findings. The transform method was used to calculate excitation profiles, and good agreement between experiment and theory was achieved when four excited electronic states were included in the calculations. In the case of TFF, a significant electronic interaction between ferrocenyl and thiosemicarbazone chromophores was observed.