Hydrogenated nanocrystalline silicon (nc-Si:H) thin film has received a great deal of attention as a promising material for flat panel display transistors, solar cells, etc. However, the multiphase structure of nc-Si:H leads to many defects. One of the major challenges is how to reduce the defects conveniently. In this work, we developed a simple and effective method to deposit low-defect-density nc-Si:H thin film. This method is simply by tuning the deposition pressure in a high-pressure range in plasma-enhanced chemical vapor deposition (PECVD) process. Microstructures of the nc-Si:H were characterized by Raman, AFM, and SEM. Furthermore, we focused on the defect density which was the key characteristic for photovoltaic materials and achieved the defect density of 3.766 × 10 16 cm −3. This defect density is lower than that of previous studies on the fabrication of low-defect-density nc-Si:H by other complex methods in PECVD process. The minority carrier lifetime of nc-Si:H is thus greatly improved. Moreover, we demonstrated the mechanism about the effect of deposition pressure on the ion bombardment and proved that the defect density is the key characteristic for nc-Si:H photovoltaic material.