Bulk polytetrafluoroethylene (PTFE) possesses excellent chemical stability and dielectric properties. Indeed, thin films with these same characteristics would be ideal for electret applications. Previously, the electret properties of PTFE-like thin films produced by rf sputtering or plasma enhanced chemical vapor deposition were found to deteriorate due to structural changes and surface oxidation. In this article, the technique of initiated chemical vapor deposition (iCVD) is evaluated for electret applications for the first time. The iCVD method is known for its solvent-free deposition of conformal, pinhole-free polymer thin films in mild process conditions. It is shown that PTFE thin films prepared in this way, show excellent agreement to commercial bulk PTFE with regard to chemical properties and dielectric dissipation factors. After ion irradiation in a corona discharge the iCVD PTFE thin films exhibit stable electret properties, which can be tailored by the process parameters. Due to the mild deposition conditions, the iCVD technique is suitable for deposition on flexible organic substrates for the next-generation electret devices. It is also compatible with state-of-the-art microelectronic processing lines due to the characteristics of conformal growth and easy scaling up to larger size substrates.