Raman, IR and NMR spectra were measured in order to elucidate the role of 4-phenyl-3-buten-2-one in zinc electroplating. First, solutions of this compound dissolved in methanol and methanol/water mixtures were studied. NMR data show that the solvation was caused by Van der Waals forces. Density functional theory calculations were performed to support vibrational wavenumber assignments of the observed bands. The studied SVWN/DN** basis set shows good agreement with the experimental results. Additionally, Raman spectra of 4-phenyl-3-buten-2-one dissolved in an electroplating bath were obtained and a red shift was observed of the carbonyl group. This effect was explained as a result of the packing density of the investigated molecule modified in the electroplating bath. No complex was detected between zinc and 4-phenyl-3-buten-2-one.