A comparative study of deposition nanocrystalline silicon (nc-Si) on various buffer layers is investigated. The nc-Si films were deposited in a hot-wire chemical vapor deposition (CVD) system. Through Hall measurement, scanning electron microscopy (SEM), atomic force microscope (AFM), Raman, and x-ray diffraction (XRD) analyses, it was found that the columnar grain (CG) size, mobility, and volume fraction of crystalline-deposited nc-Si films increase with an increase of the buffer layers’ surface roughness. The nc-Si film deposited on the nc-Si buffer layer possesses the highest Xc (volume fraction of crystalline) of 84.32%, Hall mobility of 45.9 (cm2/V s), and CG size of 200–220 nm, and it shows the strongest intensity of the XRD diffraction peak in (111).