We report the results of the low-frequency Raman experiments on CO2 which were carried out in a wide density range, along the liquid-gas coexistence curve in a temperature range of 293–303 K, and on the critical isochore of 94.4 cm3 mol–1 in a temperature range of 304–315 K. In our approach, the qualitative behavior of the diffusion coefficient D is predicted, assuming the following: first, that the low-frequency Raman spectra can be interpreted in terms of the translation rotation motions; second, that the random force could be replaced by the total force to calculate the friction coefficient; and finally, that the Einstein frequency is associated with the position of the maximum of the low-frequency Raman spectrum. The results show that the diffusion coefficient increases along the coexistence curve, and its values are almost constant on the critical isochore. The predicted values reproduce qualitatively those obtained by other techniques. The values of D were also calculated by molecular-dynamics simulation and they qualitatively reproduce the behavior of D. ©2005 American Institute of Physics