Gas-antisolvent (GAS) process using CO2 successfully prepared crystals of fullerene (C-60) from a toluene solution through a precipitation. Particle sizes of precipitated C-60 could be easily controlled by changing the initial pressurization rate of CO2, the temperature at the initial pressurization, and the quantity of C-60. Fullerene particles obtained by GAS method had regular octahedral shapes, whereas the particles obtained by adding liquid ethanol as an antisolvent to C-60 solution did not have such shape. Particle sizes could be changed in a range of 1.0-8.5 mu m by GAS method; they were wider than the range of particles obtained by ethanol addition (0.7-1.8 mu m).