The invention relates to a preparing method of self-assembly forming-dimension-controllable silicon nanocrystal films. The method mainly comprises the following steps that firstly, after the film coating pretreatment, Ar ions are used for carrying out magnetron co-sputtering on Si targets and C targets, the sputtering powers of the Si and C targets are regulated, and amorphous silicon / carbon films of a multilayer structure are alternately deposited on a silicon and glass substrate; then, the staged annealing is carried out in the nitrogen atmosphere, and the alpha-SiC / nc-Si multilayer structure films are formed. The silicon nanocrystal dimension formed by the films is controllable in a range being 2 to 10nm, meanwhile, the density of silicon nanocrystals is also controllable, and the optical band gap of the silicon nanocrystals in the range is controllably changed in a range being 2.7 to 1.8eV. The preparing method provided by the invention has the advantages that the silicon nanocrystals with the controllable dimension and density can be formed through the superlattice structure Si / C multilayer films, further, the absorption spectrum range is regulated, and in addition, the photoelectric conversion efficiency of used materials can be obviously improved. Through the films, the light absorption range and the photoelectric conversion efficiency of silicon-based photovoltaic devices are hopeful to be greatly improved.