Calcium carbonate nanoparticles of calcite structure and nanometric size were successfully synthesized by mechanochemical processing using low energy mill (100 rpm). Transmission electron micrographs demonstrated that the nanoparticles tend to form agglomerates of approximately 1 μm due to their high surface energy. A study of structure and properties of composite materials resulting from the addition of CaCO 3 nanoparticles at concentrations of 1, 2.5 and 5 wt% to epoxy resin was made. Epoxy/1 wt% CaCO 3 and epoxy/2.5 wt% CaCO 3 composites displayed an increase of 8 and 12°C in glass transition temperature (T g ), respectively. Scanning electron microscopy images of composites revealed a hierarchical structure of micrometric sized extended aggregates of nanometric calcium carbonate particles homogeneously distributed in the polymer matrix. This morphology explains the increase in hydrophobicity, as well as gains in Young's moduli, which were greater than 59% with respect to the neat epoxy as measured by Nanoindentation. Therefore, this work demonstrates that the optimum range of concentration up to 2.5 wt% of high-quality nano CaCO 3 guarantees thermal, mechanical and surface significant improvements associated with a hierarchical microstructure-nanostructure, which ultimately extend the possibilities of application of epoxy materials for nowadays challenges.