In this study, a novel mechanochemical route to prepare core-shell structured particles was introduced. XPS, TEM, and dissolving experimental results indicate the formation of [(inorganic particle)/(elastomer)] core-shell structured particles, and several kinds of calcium carbonate (nano-CaCO3) particles with various interfaces were obtained. The mechanical properties and morphological results indicate that the surface treatment of nano-CaCO, particles and the existence of outer elastic layer will strengthen the interfacial interaction between nano-CaCO, particles and PVC matrix, which results in improvement of mechanical properties of PVC/CaCO3 composites. The theoretical calculations of the interfacial interaction and DMA results confirm these especially when the surface of nano-CaCO3 particles was treated by MMA and coated in succession by ACR through vibro-milling. (c) 2006 Wiley Periodicals, Inc.