The three-phase coexisting curve of CF4 hydrate + water + fluid CF4 and laser Raman spectroscopic analysis for the CF4 hydrate system have been investigated in a temperature range of 276 to 317 K and at pressures up to 454 MPa. The present experimental results show that the CF4 molecule is able to occupy both the S- and M-cages in the high-pressure region (above 70 MPa) similar to the cyclopropane hydrate system. The pressure independence of the intermolecular O-O vibration reveals that the CF4 hydrate cage is hardly shrunk by pressurization.