We present a systematic study on the correlation of hydrogen dilution profiles to structural properties materials and solar cell performance in nc-Si:H solar cells. We deposited nc-Si:H single-junction solar cells using a modified very high frequency (VHF) glow discharge technique on stainless steel substrates with various profiles of hydrogen dilution in the gas mixture during deposition. The material properties were characterized using Raman spectroscopy, X-TEM, AFM, and C-AFM. The solar cell performance correlates well with the material structures. Three major conclusions are made based on the characterization results. First, the optimized nc-Si:H material does not show an incubation layer, indicating that the seeding layer is well optimized and works as per design. Second, the nanocrystalline evolution is well controlled by hydrogen dilution profiling in which the hydrogen dilution ratio is dynamically reduced during the intrinsic layer deposition. Third, the best nc-Si:H single-junction solar cell was made using a proper hydrogen dilution profile, which caused a nanocrystalline distribution close to uniform throughout the thickness, but with a slightly inverse nanocrystalline evolution. We have used the optimized hydrogen dilution profiling and improved the nc-Si:H solar cell performance significantly. As a result, we have achieved an initial active-area cell efficiency of 9.2% with a nc-Si:H single-junction structure, and 15.4% with an a-Si:H/a-SiGe:H/nc-Si:H triple-junction solar cell structure.