Hydrogenated silicon (Si:H) films near the threshold of crystallinity were prepared by very high-frequency plasma-enhanced chemical vapor deposition (VHF-PECVD) using a wide range of hydrogen dilution R H=[H 2]/[SiH 4] values of 2–100. The effects of H dilution R H on the structural properties of the films were investigated using micro-Raman scattering and Fourier transform infrared (FTIR) absorption spectroscopy. The obtained Raman spectra show that the H dilution leads to improvements in the short-range order and the medium-range order of the amorphous network and then to the morphological transition from amorphous to crystalline states. The onset of this transition locates between R H=30 and 40 in our case, and with further increasing R H from 40 to 100, the nanocrystalline volume fraction increases from ∼23% to 43%, and correspondingly the crystallite size enlarges from ∼2.8 to 4.4 nm. The FTIR spectra exhibit that with R H increasing, the relative intensities of both the SiH stretching mode component at 2100 cm −1and wagging mode component at 620 cm −1 increase in the same manner. We assert that these variations in IR spectra should be associated with the formation of paracrystalline structures in the low H dilution films and nanocrystalline structures in the high H dilution films.