Nonthermal plasmas generated under atmospheric pressure (AP) have been receiving increased attention in direct plasma technology applications for thin film deposition. This is because the atmospheric-pressure plasma-enhanced chemical vapor deposition (AP-PECVD) is expected to realize low-cost and high-throughput processing with open air systems, which are of prime importance for various industrial applications. A large number of studies have been reported on the preparation of thin films using various types of AP plasma sources such as corona, dielectric barrier and AP glow discharges excited by pulsed or low-frequency power sources that can produce a nonequilibrium AP plasma. Most of the reported films using these common AP plasma sources have been related to polymers, oxides, and carbon materials. On the other hand, by virtue of the low ion energy due to the high collision frequency, AP-plasma process can have a nature of soft or gentle processing in addition to high-rate processing. Therefore, AP-PECVD also has a potential to form good-quality functional thin films, such as high-purity semiconductor or insulator thin films, which may be applicable for electronic devices. Although the development of AP-PECVD technology for such applications are attractive in the future advanced industry, the reports on these applications are limited. The reason may be related to the fact that the high collision frequency in AP plasma enhances secondary reactions in the gas phase to generate dust particles which will deteriorate the film quality, and also limits mass transport, which leads to poor uniformity of the resulting film. In the present article, the authors review the present status of AP low-temperature plasma processes, bearing in mind their application for high-purity functional thin films including silicon and related materials. The authors first summarize recent progress in the use of common AP plasma sources for direct PECVD processes. To grasp the present status of AP-PECVD technique, the authors have picked up popular materials for AP-PECVD, such as carbon, oxides, and other inorganic materials as well as silicon and related materials. Although there already exists a plenty of good review articles dealing with PECVD using common AP plasma sources, works on reviewing PECVD using radio-frequency (RF) and very-high-frequency (VHF) excitations of AP plasma seem to be insufficient. RF and VHF excitations of AP plasma are capable of generating continuous oscillating glow discharges without unstable streamers and filaments, which will be important to form uniform and dust-free films. So, secondly, the authors discuss the key distinguishing features of PECVD using RF and VHF excitations of AP plasma from the common AP plasma sources. Finally, they describe examples of the application of AP-VHF plasma to the preparation of silicon and related thin films.