High breakdown strength and low dielectric loss are necessary for the outdoor insulator using silicone rubber (SR) composites. In this work, polydopamine coated mica (mica-PDA) was synthesized via bioinspired dopamine self-polymerization, and mica-PDA-filled SR composite (SR/mica-PDA-VTMS) was prepared using vinyl tri-methoxysilane (VTMS) as a silane coupling agent which serves as the molecular bridges between the organic rubber and the inorganic filler. The SR/mica-PDA-VTMS composite demonstrated dense and uniform morphology where the filler was well dispersed. Due to the strong interfacial interactions between filler and rubber, the SR/mica-PDA-VTMS composite exhibits much lower dielectric loss compared to the other mica-filled SR composites, which was comparable to the prepared alumina-tri-hydrate-filled SR composites. Moreover, the breakdown strength of ~31.7 kV/mm and tensile strength of 5.4 MPa were achieved for the SR/mica-PDA-VTMS composite, much higher than those of the other as-prepared SR composites.