Surface modification of CaCO3 nanoparticles treated by methyltrime-thoxysilane (MTMS) has been studied and the effect of this on foam and emulsion stability has been investigated. The surface modification of CaCO3 nanoparticles by MTMS was confirmed by measurements of FT-IR, DSC, XRD, TGA and XPS analysis. Floating test and contact angle measurement have also been conducted to study the effect of hydrophobicity of particles. In modified CaCO3 nanoparticle-surfactant mixture, foam stability has improved compared to a surfactant-only system. Investigation into the influence of the wettability, nanoparticle CaCO3 particles on the type and stability of water-decane emulsions is described. With the increase of the MTMS concentration, CaCO3 nanoparticles changed from hydrophilic to hydrophobic, and water-in-oil (W/O) emulsions were obtained. The adsorption of CaCO3 nanoparticles at the surface of emulsion droplets was observed by High Resolution Fluorescence microscopy.