Silicon nitride (Si3N4) and silica (SiO2) thin films are of interest for applications in microelectronics and optics. Non-hazardous alternatives to silane (SiH4) as the silicon precursor in the chemical vapor deposition (CVD) of these materials are an attractive target for research. It is shown that pentamethylcyclopentadiene-substituted silanes offer the opportunity to tailor precursors for particular CVD requirements.