The infrared and Raman spectra of 2-acetylpyrrole dissolved in various solvents, are reported in addition to the Raman spectra of the solid state at pressures up to 30 kbar. The high-pressure behaviour of the Raman-active N-H bands shows beyond any doubt that hydrogen bonded species exist in solid 2-acetylpyrrole, but these results could not distinguish between intra- or intermolecular bonds. Evidence of hydrogen bonded species was also found in solutions of 2-acetylpyrrole in addition to vibrations which point to the existence of ‘free’ oranti-bonded molecules. The hydrogen bonded species existing in solutions and in the solid state appear to be identical.