Silicones have a long history of use in biomedical devices, with unique properties stemming from the siloxane (Si-O-Si) backbone that feature a high degree of flexibility and chemical stability. However, surface, rheological, mechanical, and electrical properties of silicones can limit their utility. Successful modification of silicones to address these limitations could lead to superior and new biomedical devices. Toward improving such properties, recent additive strategies have been leveraged to modify biomedical silicones and are highlighted herein.