In this work, hybrid fillers consist of modified silica (SiO2) and multiwalled carbon nanotube (MWCNT) were used to improve the mechanical, dielectric, and thermal properties of fluorosilicone (FSR) composites via a direct mechanical mixing method. With the increase of CNT loading in SiO2/CNT hybrid loading ratio, the tensile properties, dielectric constant, electrical conductivity, and thermal properties all increase without a sharp sacrifice of flexibility. The dielectric constant of FSRâS15/C5 achieved 7,370 @1âkHz, which is about four orders of the FSRâS20, and the dielectric loss remains as low as 0.676 @1âkHz. Therefore, the linkage of SiO2 and FSR chains not only enhances the interfacial interaction between the fillers and FSR matrix but also decreases the agglomeration of the fillers in matrix. What is more, modified SiO2 and CNT were designed as the effective hybrid filler to improve the performance of the polymeric matrix through synergic effect.