Silicone rubber composites with good comprehensive properties modified with polyurethane were obtained through mixing and vulcanizing methods. Firstly, the polyurethane prepolymer with double bonds was prepared by polytetrahydrofuran glycol (PTMG, Mn = 1000), isophorone diisocyanate (IPDI), and 2-hydroxyethyl methacrylate (HEMA). The prepolymer was then added to the silicone rubber compounds to prepare silicone rubber composites, combining the excellent properties of polyurethane with the silicone rubber materials. The effects of polyurethane content on the mechanical properties, insulation, hydrophobicity, thermal stability, and flame retardancy of composites were studied in detail. The results showed that the silicone rubber composites not only have good hydrophobicity, thermal stability and flame retardant properties, but the addition of polyurethane significantly improves the tensile strength at room and low temperatures and the volume resistivity of the materials. The tensile strength increased by 32.5%, and the volume resistivity nearly doubled. The excellent electrical insulation, high hydrophobicity and good mechanical properties make the silicone rubber composites appropriate for use in the field of polymeric house arresters.