Spin-on Low-K materials are potentially very attractive as interconnection materials in a wide range of semiconductor structures. In this work, new organic-inorganic hybrid materials synthesized by vinylsilane polymerization were proposed. According to compositions and additional fabrications, dielectric constants of these materials were evaluated to be 2.3∼3.1. The hardness was 2.0GPa after 430°C curing. These materials had good adhesion strength such that fracture toughness on silicon wafer was 0.22 MPam0.5 without any adhesion promoters. This result indicates that these organicinorganic hybrid materials are very promising candidates for low-K dielectrics.