In this paper, the surface tension components of three silicone resins were determined with an advanced contact angle technique, which was composed of dynamic cycling contact angle and axisymmetric drop shape analysis (ADSA). The interfacial properties of three silicone/quartz glass fiber composites were measured through interfacial shear strength (IFSS) testing experiment. It was found that the Lifshitz–van der Waals component was the main surface tension component for all of the silicones. There is a perfect linear relationship between the interfacial tension and the IFSS. With the increase of the Lifshitz-van der Waals component, the interfacial tension and the IFSS of composites increased. Therefore, the Lifshitz-van der Waals component is the most important parameter for explaining the interfacial shear property of silicone/glass fiber composites.