Hybrid materials prepared from single-walled carbon nanotubes (SWNTs) and organosilicon compounds, which exhibit excellent field emission efficiency, are discussed. The covalent combination of C60 and organosilicon compounds produces a new class of silylfullerene. The combining π and σ conjugated compounds exhibit interesting characteristics, and the silylfullerene has lower oxidation and higher reduction potential than the analogous carbon substituted derivatives and C60 itself. This unique electrochemical property is the electron-releasing nature of silicon relative to carbon. The physiosorption of organosilicon compounds on the surface of SWNTs is also effective for improvement of the field emission properties of SWNTs. The hybrid materials of SWNTs with organosilicon compounds are not sensitive to the oxidation potential of the organosilicon compounds. This modification suggests a great potential of industrial utilization for field emission sources.