- Silicone hydrogel contact lenses (CLs) permit increased oxygen permeability through their incorporation of siloxane functional groups. However, contact lens biofouling can be problematic with these materials; surface modification to increase lens compatibility is necessary for acceptable properties. This work focuses on the creation of an antifouling CL surface through a novel grafting method. A polymer incorporating 2-methacryloyloxyethyl phosphorylcholine (MPC), well known for its antifouling and biomimetic properties, was grafted to the model lens surfaces using surface-initiated atom transfer radical polymerization (SI-ATRP). The SI-ATRP modification generated a unique double-grafted polymeric architecture designed to resist protein adsorption through the presence of a surrounding hydration layer due to the PC groups and steric repulsion due to the density of the grafted chains. The polymer was grafted from model silicone hydrogel CL using a four-step SI-ATRP process. Attenuated total reflectance-Fourier transform infrared spectroscopy and XPS were used to confirm the surface chemical composition at each step of the synthesis. Both the surface wettability and equilibrium water content of the materials increased significantly upon polyMPC modification. The surface water contact angle was as low as 16.04 ± 2.37° for polyMPC-50 surfaces; complete wetting (∼0°) was observed for polyMPC-100 surfaces. A decrease in the protein adsorption by as much as 83% (p < 0.000 36) for lysozyme and 73% (p < 0.0076) for bovine serum albumin was observed, with no significant difference between different polyMPC chain lengths. The data demonstrate the potential of this novel modification process for the creation of extremely wettable and superior antifouling surfaces, useful for silicone hydrogel CL surfaces.