A new CaCO3-SiO2 composite with core-shell structure was successfully prepared by mechano-chemistry method (MCM). SEM and FTIR indicated that SiO2 particles were homogeneously immobilized on the surface of CaCO3. The well dispersion of this CaCO3-SiO2 composite into silicone rubber can not only reduce the usage amount of SiO2, but also improve the mechanical properties of silicone rubber. By the calculation, the theoretical numbers of the SiO2 particles is about 10 times as large as that of CaCO3 particles in the CaCO3-SiO2 composite. Mixing CaCO3-SiO2 composite in silicone rubber can enhance the breaking strength of the silicone rubber about 18% as high as that when mixing the pure SiO2. And the elongation at break is about 14% less than that of adding the pure SiO2 sample.