The compilations of fundamental vibrational frequencies of molecules previously published as NSRDS—NBS—6, NRSD—NBS—11, NSRDS—NBS—17, and NSRDS—NBS—39, are extended to 58 additional molecules. Selected values of the fundamental vibrational frequencies are given for each molecule, together with observed infrared and Raman spectral data and citations to the original literature. The selection of vibrational fundamentals has been based on careful studies of the spectral data and comprehensive normal‐coordinate analyses. An estimate of the accuracy of the selected values is included. The tables provide a convenient source of information for those who require vibrational energy levels and related properties in molecular spectroscopy, thermodynamics, analytical chemistry, and other fields of physics and chemistry.