A 30-nm-thick Ni layer was deposited on top of the nc-Si:H (hydrogenated nanocrystalline Si) films by rf-magnetron sputter, and then heat-treatments were carried out at temperatures of 350–500∘C. Si nanocrystallites were formed in the Ni/nc-Si:H bilayer films during the post-deposition heat-treatments. The intensity of the photoluminescence spectra of the post-deposition heat-treated films gradually increased at wavelengths of ∼420 as well as ∼580 nm with raising the annealing temperature from 350 to 500∘C. It is highly likely that the increase of the photoluminescence intensity is caused by the increase in the total volume of the nanocrystallites in the films. It was found that the nickel-induced crystallization processing enhanced the formation of Si cystallites with the size of ∼2 and ∼5 nm in the films.