Provided is a method of forming a polycrystalline silicon thin film with improved electrical characteristics. The method includes forming an amorphous silicon thin film on a substrate, partially melting a portion of the amorphous silicon thin film by irradiating the portion of the amorphous silicon thin film with a laser beam having a low energy density, forming polycrystalline silicon grains with a predetermined crystalline arrangement by crystallizing the partially molten portion of the amorphous silicon thin film, completely melting a portion of the polycrystalline silicon grains and a portion of the amorphous silicon thin film by irradiation of a laser beam having a high energy density while repeatedly moving the substrate by a predetermined distance, and growing the polycrystalline silicon grains by crystallizing the completely molten silicon homogeneously with the predetermined crystalline arrangement.