AbstractTo realize the great potential of silicone rubber in advanced electronics, high dielectric constant and low loss tangent are currently pursued. Adding a third phase to conductive filler/silicone rubber composites may enhance the properties of the composites, but the appropriate particle size of the third phase is an open question. Here, MoS2 was used as the third phase to prepare the Ti3C2Tx MXene/MoS2/methylvinyl silicone rubber (VMQ) ternary composites, and the influence of different sizes of MoS2 (200 nm and 2 μm) on the dielectric performance of the composites was investigated. The dielectric constant of the Ti3C2Tx MXene/VMQ composites with 5 wt% MoS2 nanoparticles shows a 279% enhancement from 2.78 to 7.75 at 103 Hz, better than that of the Ti3C2Tx MXene‐MoS2 hybrid fillers/VMQ composites. Compared with micron MoS2, nano MoS2 can significantly enhance the dielectric performance of conductive filler/polymer composites because of shorter interparticle distances and enhanced interfacial polarization. Meanwhile, the composites exhibit low loss tangent (lower than 0.0015) and good thermal stability (up to 400°C) because of the low filling amounts of Ti3C2Tx MXene and MoS2 nanoparticles. Excellent flexibility with Young's modulus of 285 kPa and elongations break of 446% was also obtained. The design of these ternary composites greatly improves the dielectric and mechanical properties, which means that the dielectric material has a broad application prospect in modern electronics industry.Highlights High dielectric constant was gained in Ti3C2Tx MXene/5n‐MoS2/VMQ composites. The MXene/5n‐MoS2/VMQ composites exhibited excellent mechanical properties. Appropriate filler size can benefit the performance of polymer composites.