Silicone rubber (SR), a material widely used in the biomedical field, was modified with stimuli-responsive poly(N-vinyl caprolactam) (PVCL) and poly(methacrylic acid) (PMAA) with the aim of improving its ability to host drug molecules. The grafting of PVCL and PMAA onto SR was carried out by means of a c-ray preirradiation method, and the dependence of the grafting yield on the comonomer concentration, preirradiation dose, temperature, and reaction time was evaluated. Modified SR films were characterized by Fourier transform infrared spectroscopy, differential scanning calorimetry, thermogravimetric analysis, and swelling studies to confirm the grafting of the copolymer. The SR-g-[vinyl caprolactam (VCL)/methacrylic acid (MAA)] copolymers showed a sensitivity to the temperature and pH, high hemocompatibility, and low affinity to bovine serum albumin and fibrinogen proteins. Moreover, the SR-g-(VCL/MAA) copolymers were able to host some nonsteroidal anti-inflammatory drugs, such as diclofenac and ibuprofen, and the antifungal agent nystatin. The graft copolymer was shown to be useful for providing sustained release for several hours; this indicates that the modified SR is a promising material for drug-eluting medical devices. V C 2015 Wiley Periodicals, Inc. J. Appl.Polym. Sci. 2015, 132, 41855.