Nanocomposites of layered silica nanoparticles (LSN) obtained by the sol-gel method, and commercial montmorillonite clay Cloisite((R))20A with polypropylene (PP) and Cloisite((R))30B with polyamide-6 (PA6) were prepared by melt blending in order to study their effects on barrier, mechanical properties, and thermal stability. Transmission electron microscopy (TEM) showed that all of the nanocomposites present agglomerated nanoparticles with some degree of individual particles. In barrier properties, LSN dramatically increased the oxygen and water vapor permeability of PP at low loadings (<5 wt %) due to the percolation effect. However, in PP and PA6 nanocomposites with clays, the permeability showed increases and decreases depending on the solubility of the permeating gases with the clays and the polymers. Tensile stress-strain tests otherwise showed that the nanocomposites with clays present an enhancement in the elastic modulus. Meanwhile, with the LSN, a decrease was found due to the formation of agglomerations and voids. Finally, thermogravimetric analysis under inert conditions showed the nanoparticles do not have a significant effect on the thermal stability of the nanocomposites. These results expose the relevance of the type of layered nanoparticle and polymer matrix on the barrier, mechanical, and thermal behaviors of the resulting nanocomposites.