Controlling the surface characteristics of inorganic materials with an organic shell is of great interest for control of the properties of the final material. A challenge is thus to be able to deposit a polymer shell with different solvation properties onto the surface of inorganic particles and to have a good control of the thickness of the organic layer without a prefunctionalization of surfaces. We demonstrate, in this paper, a method for coating silica particles (170-550 nm), used as model substrates, with either a hydrophilic (polyethylene glycol) or a hydrophobic polymer (polybutadiene hydroxy terminated) using a supercritical antisolvent process (precipitation from a compressed antisolvent). Several operating parameters were studied to control precisely the thickness of the deposited layer (from 2 to 30 nm), which was characterized using TEM, FESEM, XPS, and UV-visible techniques. This work demonstrates that supercritical antisolvent processes are powerful methods and good alternatives to conventional coating techniques toward the development of hybrid and/or core-shell nanomaterials.