Polymer nanocomposite based on layered structure such as graphene, MoS2, MoO3 and WS2 has become an active field of research due to their exceptional thermal, mechanical and electrical properties. Achieving uniform dispersion of layered nanostructures within the polymer matrix is challenging because of the agglomeration of nanostructures which occurs due to the Van der Waals attraction and the cohesive nature between the two phases. In this work, we report the preparation of PVDF-modified MoS2 nanocomposites by the solvent blending method. The XRD results reveal the interaction of the negatively charged surface of MoS2 sheets and the positive CH2 group of PVDF through the predomination of beta-phase. Morphological observation through SEM suggests the MoS2 induced formation of nanofibres in the composite. Enhancement in the thermal stability of the nanocomposite is observed and is possibly due to the heat barrier by the exfoliated MoS2 which in turn supports the tortuous effect. The DSC of the PVDF-modified MoS2 composite indicates the domination of beta-phase and the hindrance to crystallization of PVDF. Improvement in the mechanical strength of the composites was also noticed on higher filler concentration.