Resonance Raman spectra and band assignments of some phenylhydrazonopropanedinitriles, including the 3-chloro and the 2-carboxy derivatives, in the 900–2300 cm−1 spectral range are presented and discussed. I5N and 2H isotopic shifts have been used to clarify the assignments, which have been made for both protonated and deprotonated forms of the compounds. The resonance Raman spectra of the protonated forms show strong coupling between NH deformation and hydrazone vibrations. This coupling is lost in the anionic forms, which are considered to have considerable carbanion character. By using the drastic changes between the resonance Raman spectra of protonated and deprotonated forms, the pKa value of the 2-carboxy derivative has been determined.