Deposition phase diagrams are convenient for categorizing the evolution of the surface microstructure and phase with accumulated thickness for hydrogenated silicon (Si:H) films during plasma-enhanced chemical vapor deposition (PECVD). They can also be used to assess the electronic quality and device suitability of Si:H, based on previous correlations. In this study, phase diagrams have been applied in a comparison of Si:H PECVD using two different plasma excitation frequencies (rf: 13.56 MHz; and vhf: 60 MHz). Smooth crystalline Si (c-Si) wafer substrates have been used to obtain the surface roughness evolution with maximum sensitivity in the amorphous silicon (a-Si:H) growth regime. This study has shown that under all explored conditions of plasma power, frequency, and gas pressure, yielding deposition rates of 0.5-20 Å/s, a-Si:H exhibits improved microstructural characteristics with increasing H2-to-SiH4 flow ratio R right up to the amorphous-to-(mixed-phase microcrystalline) [a→(a+μc)] boundary of the phase diagram. For depositions at R values much lower than the a→(a+μc) transition for a thick film, vhf PECVD can provide a significant improvement in microstructural evolution over rf PECVD, for a given deposition rate. For optimum R just below the a→(a+μc) transition, however, vhf and rf a-Si:H films exhibit remarkably similar structural evolution for a given rate.