There is a growing demand for a high voltage silicone rubber composite with high mechanical property and high electrical property. The effect of modified cross-linking agent on the mechanical, electrical properties, and short-circuit test performance of silicone rubber insulators have been investigated. To use base polymer, the various silicone polymers were prepared by the equilibrium polymerization. Aluminum trihydrate surface was treated by vinyl silane. Liquid silicone rubber nanocomposite was prepared from the compounding of VPMPS, HPDMS, catalyst, and alumina trihydrate modified with 1,3,5-trivinyl-l,3,5-trimethylcyclotrisiloxane. The mechanical property and electrical property for insulation materials were measured, indicating the high tensile strength and the good short-circuit property.