Hydrogenated microcrystalline silicon films (μc-Si:H) deposited at high deposition rates (∼2 nm/s) by means of the very-high-frequency (VHF) deposition technique in the high pressure depletion regime have been integrated into single junction p-i-n solar cells. It is demonstrated that μc-Si:H solar cells can be optimized using a twofold approach. First the bulk properties, deposited under steady-state plasma conditions, are optimized by monitoring the presence of crystalline grain boundaries in μc-Si:H. These hydrogenated crystalline grain boundaries can easily be detected via the crystalline surface hydrides contribution to the narrow high stretching modes by infrared transmission spectroscopy. The crystalline grain boundaries suffer from postdeposition oxidation which results in a reduced red response of the solar cell. The absence of these crystalline surfaces in an as-deposited μc-Si:H matrix reflects the device grade microcrystalline bulk material. Second, the prevention of silane backdiffusion from the background during the initial growth is a necessity to deposit a uniform μc-Si:H phase over the entire film thickness. The initial growth is optimized while preserving the optimized bulk properties deposited under steady-state conditions, using initial profiling of plasma parameters such as the silane flow and the VHF power density. Solar cell devices with efficiency of 8.0% at a μc-Si:H deposition rate of 2.0 nm/s are obtained using the presented approach.