Poly(vinylidene fluoride) (PVDF) and its copolymers are known for possessing the highest electroactive response including dielectric constant, piezoelectric and ferroelectric effects which has a wide range of applications such as in energy transfer, energy generation and storage, monitoring and control, and include the development of capacitors, sensors, actuators and so on. We report an enhancement in dielectric properties in PVDF generated by the addition of MoS2 nanosheets. The addition of 1 wt% MoS2 nanosheets as a filler in PVDF, stabilize its beta phase over the alpha phase, resulting in a significant increase in dielectric constant (ε’) across a wide range of frequencies (100 Hz to 1 MHz) and temperatures (140 K- 340 K). The high dielectric constant was achieved by the PVDF-MoS2 nanocomposite while maintaining a relatively low tangent loss factor of 0.94. Such properties in soft polymer-based piezoelectric materials were previously challenging and unachievable. The nanocomposite exhibits excellent ferroelectric properties with 11 times enhancement in remnant polarization compared to pristine PVDF in ambient conditions. The stored energy density (Us) is 39.43 mJ/cm3 for the PVDF-MoS2 film. These lead-free and soft polymer-based nanocomposites can bring remarkable advances in various flexible sensors, data storage, and energy harvesting applications.