To study the feasibility of using supercritical CO2 to concentrate natural tocopherols from soybean oil deodorizer distillate (DOD), we measured the ternary phase equilibrium data for methyl oleate + alpha-tocopherol + supercritical CO2 from (313.15 to 353.15) K in the pressure range from (10 to 29) MPa. The measured data were well correlated using the Soave-Redlich-Kwong EOS with the Adachi-Sugie mixing rule. The separation factor between methyl oleate and tocopherol in CO2 was investigated. On the basis of these results, equilibrium lines in the experimental ranges were obtained that provide fundamental data for concentrating tocopherols with supercritical CO2. In addition, because the distribution of tocopherol in supercritical CO2 increases markedly because of the abundance of methyl oleate, methyl oleate was shown to act as a cosolvent for tocopherol. Finally, according to the obtained results, a strategy for a separation operation was suggested. Visual observation also provided information useful in further experiments and design.