Comparison of the observed and calculated vibrational frequencies of all-trans-octatetraene indicates that the density functional theory (DFT) using Becke's exchange and Lee-Yang-Parr's correlation functionals is as accurate as the Hartree-Fock (HF)-based scaled quantum mechanical force field approach in predicting fundamental vibrational frequencies. As the DFT calculation does not use any empirical parameters pertaining to the subject molecule and its computational cost scales more favorably than that of the HF theory, it is a more promising approach to molecular vibrational problems and should replace the empirical normal coordinate analysis for assisting vibrational assignments.