Fluorosilicone polymers combine the properties of both fluorocarbons and siloxanes, yielding materials with unique properties. Novel crosslinked fluorosilicone polymers were synthesized by grafting diisocyanate-terminated polydimethylsiloxane (PDMS) to hydroxyl-functionalized fluoropolymers of poly(tetrafluoroethylene-co-vinyl acetate-co-vinyl alcohol) (PTFE-VAc-VA), as confirmed by elemental bulk and surface analysis. The fluorosilicone polymers containing 34 mol% of TFE were thermally stable with a degradation temperature of 267 °C. Fluorosilicone films were found to be more hydrophobic than the parent, non-grafted fluoropolymers; dynamic advancing and receding water contact angles for PTFE-co-VAc-co-VA-g-PDMS were 104° ± 1° and 61° ± 1°, respectively, whereas for PTFE-co-VAc they were 90° ± 2° and 59° ± 2°. The combined properties of thermal stability and hydrophobicity suggest that these fluorosilicones may be useful for coating and paint applications.Key words: fluoropolymers, fluorosilicone, polydimethylsiloxane, supercritical carbon dioxide.