The hydrosilylation approach to silicone aerogels synthesis in supercritical CO2 was thoroughly investigated in this work. Commercially available functionalized PDMS was used as a hydride-containing component that was cross-linked using a set of PDMS-based divinyls with various lengths. It was demonstrated that when the density of the CO2 is close to that of the reagents, monolithic aerogels are formed. Varying the CO2 density and the length of a divinyl component, one can obtain flexible hydrophobic aerogels with densities as low as 0.13 g/cm(3) or fine porous microgranules of about 0.5 mm diameter.