Among various elastomers, polydimethylsiloxane is versatile owing to exotic compilation of properties such as low temperature flexibility, high thermal stability, incredible surface properties and even excellent biocompatibility. However, it finds limited use in some instances where strength is a critical parameter. Hence, this work aims at improving the mechanical and dynamic mechanical of the vulcanizates by integrating various fibrous nanofillers of organic and inorganic origin. In this piece of work, four different nanofiller systems viz., sepiolite, carbon nanofiber, hydroxyapatite and fibrous nanosilica as the reinforcing agent were compared. We pursued the nanocomposite preparation through in situ polymerization technique. Dispersion was found to be an important aspect which governed the property enhancement of the nanocomposites. The extent of dispersion of the various nanofillers was inspected through morphology analysis by High Resolution Transmission Electron Microscopy (HRTEM) studies. These results were correlated with the improvement of tensile strength, tensile and storage modulus of the nanocomposites and explained in terms of increased interaction of the hybrid materials, due to collective non-bonding forces of attraction (such as hydrogen bonding) between the components.