This study investigates the properties of polydimethylsiloxane (PDMS)‐based nanocomposites with different loadings of two‐dimensional molybdenum disulfide (MoS2) nanosheets. The uniform incorporation of the MoS2 nanosheets in the PDMS matrix was confirmed by unique excitonic absorption peaks, Raman signatures, and x‐ray photoelectron spectra of the MoS2. Owing to the excellent mechanical properties of the embedded MoS2 nanosheets, the elastic modulus and tensile strength of PDMS respectively increased to 42.86% and 19.63% compared to that of pristine PDMS, even at a low MoS2 loading of 0.04 wt%. A dynamic mechanical analysis of the nanocomposites revealed an increase in the storage modulus of PDMS by 9.83% and 30.88% with 0.04 wt% MoS2 loading at strain and frequency sweeps from 0% to 1% and 0.01–10 Hz, respectively. The low MoS2 loading also increased degradation temperature for 50% weight loss from 575.76 (for PDMS) to 652.74°C (for MoS2‐PDMS). In addition, ball‐on‐disk tribology tests revealed that the incorporation of MoS2 nanosheets withstand higher angular speeds (up to 15.71 rad/s) and significantly reduced the friction coefficient by 39.69% (at 7.85 rad/s). Our results imply that MoS2‐PDMS nanocomposites could potentially be used in various applications that require dielectric properties with improved mechanical and thermal stability.