The samples of radiationally linked vinyl (1%) methylsilicone elastomer (silicone) were modified in glow-discharge air plasma. Surface relaxation was studied by the data on equilibrium contact angles. The degree of relaxation is shown to increase with increasing plasma treatment duration, probably due to the increase in the destruction degree of the spatial network of chemical bonds in the silicone surface layer. The changes in the chemical com position of the surface were controlled using attenuated total reflectance-infrared spectroscopy. Plasma treatment leads to increase of the polar component of the polymer surface energy and increase of the absorption bands of carboxyl and hydroxyl groups in its spectra. These characteristics disappear when the samples are kept in the open air and can be recovered by putting them into water. Such behavior can be explained by the fact that the polar oxygen-containing groups, forming on the surface due to plasma treatment, pass inside the polymer. Considering the adhesion properties of modified silicone, its biocompatibility was predicted.