PVC/CaCO3 polymer nanocomposites of differing compositions were produced using a two-roll mill and compression molding. The morphology was observed using transmission electron microscopy, and the static and dynamic mechanical and fracture properties determined. The presence of nanometer-sized CaCO3 particles led to a slight decrease in the tensile strength but improved the impact energy, the storage modulus and the fracture toughness. Fracture surface examination by scanning electron microscopy indicated that the enhanced fracture properties in the nanocomposites were caused by the assisted void formation at the particles. This hypothesis is supported by a microstructure-based finite element modeling based upon elastic–plastic deformation around a weakly bonded particle. Hence, this provides an explanation of both the uniaxial tensile behavior and enhanced toughness of the nanocomposites.