In situ high pressure Raman spectra of tetramethylurea have been measured up to 25 GPa, liquid-solid and solid-solid phase transitions were detected at 0.2 GPa and 7.4 GPa, respectively. An unprecedented spectral phenomenon is the observation of a Fermi resonance between the fundamental modes. An exponential relationship between the intensity and the frequency difference was concluded. Pressure provides us a new way to study the correlation between Fermi resonance parameters.