The influence of the Si-based crystallization precursor on the quality of the resulted poly-Si crystallized by 2ω YAG laser was investigated in this paper. Based on the simulation analysis, we suggested that the H content in crystallization precursor maybe one of main effect factors. It has been found that the lower H content in Si-based precursor, the better crystallinity of the resulted poly-Si is. By using the low H content Si-based film as the precursor, the poly Silicon with the grain size of about 500 nm crystallized by 2ω YAG was obtained at the relatively optimal crystallization conditions. Meanwhile, a dehydrogenation process before laser crystallization also could be omitted. It would be beneficial to lower cost of crystallization of a-Si.