AbstractThe lattice vibrational spectrum ofp‐nitrotoluene (PNT) single crystals has been studied by Raman and IR spectroscopic techniques. Twenty‐one lines have been recorded in the Raman spectrum and nine lines in the far IR spectrum. Calculations of vibrational frequencies have been performed using the rigid molecule approximation. Intermolecular interactions have been described by atom‐pair intermolecular potential functions for interatomic distances up to 4.0 Å. An assignment of the observed to the calculated frequencies has been pr