Hydrogenated nanocrystalline silicon (nc-Si:H) is a promising alternative for crystalline silicon (c-Si) in the photovoltaic industry. We proposed an atmospheric pressure thermal plasma enhanced CVD (APTPECVD) process for high rate deposition of nc-Si:H on silicon and glass substrates using SiCl4 as the deposition precursor. The deposition rate under typical operating conditions could reach 9.78 nm s−1, and the deposited nc-Si:H film thickness could reach 17.6 μm. The grain diameter and crystalline fraction of the deposition product were characterized using SEM, TEM, Raman spectroscopy and XRD. The photoluminescence performance at room temperature was discovered.