With the miniaturization and integration of electronic components in wireless communication and wearable devices, the demand for low-cost flexible composites with temperature-stable high dielectric constant and low loss has substantially increased. However, such comprehensive properties are fundamentally difficult to combine for conventional conductive and ceramic composites. Here, we develop silicone elastomer (SE) composites based on hydrothermally grown MoS 2 on tissue paper-derived cellulose carbon (CC). Such design promoted the formation of microcapacitors, multiple interfaces, and defects reinforcing interfacial and defect polarizations and resulting in a high dielectric constant of 9.83 at 10 GHz with low filler loading of 15 wt %. Unlike highly conductive fillers, MoS 2 @CC with low conductivity ensured a very low loss tangent of 7.6 × 10 −3 , which was also influenced by the filler dispersion and adhesion to the matrix. Apart from breaking the typical conflict between high dielectric constant and low losses of traditional conductive composites, MoS 2 @CC SE composites were highly flexible with temperature-stable dielectric properties making them attractive as flexible substrates in microstrip antenna applications and extreme environment electronics. Moreover, recycling from waste tissue paper makes them potential candidates as low-cost and sustainable dielectric composites.