A kind of hydrogenated diphasic silicon films has been prepared by a new regime of plasma enhanced chemical vapor deposition (PECVD) near the phase transition regime from amorphous to nanocrystalline. The microstructural properties of the films have been investigated by the micro-Raman and Fourier transformed Infrared (FT-IR) spectra and atom force microscopy (AFM). The obtained Raman spectra show not only the existence of nano-scaled crystallites, but also a notable improvement in the medium-range order of the diphasic films. For the FT-IR spectra of this kind of films, it notes that there is a blueshift in the Si-H stretching mode and a redshift in the Si-H wagging mode in respect to that of typical amorphous silicon film. We discussed the reasons responsible for these phenomena by means of the phase transition, which lead to the formation of a diatomic hydrogen complex, H2* and their congeries.