Manipulating dielectric properties of polydimethylsiloxane (PDMS) is an important consideration for flexible, low-loss device design. This paper presents a method for reducing dielectric loss (tan δ) by forming PDMS composites loaded with various concentrations of either alumina (Al2O3) or polytetrafluoroethylene (PTFE) particles. The structural, mechanical, and electrical properties of the composites are investigated. Theoretical mixing models were used to predict the relative permittivity (εr) of PDMS composites, and good similarity with the measured εr was observed. The incorporation of either low dielectric loss filler in the PDMS matrix (up to 50 wt. % filler loading) is shown to reduce the dielectric loss while maintaining the flexibility of the host matrix. The fillers can also control the permittivity of the composite, either increasing or decreasing relative permittivity from that of PDMS. Interestingly, a strain of ∼500% can be applied to 15 wt. % PDMS/PTFE composites, compared with ∼350% for pure PDMS.