A 532 nm Nd-YAG laser was applied to crystallize amorphous Si thin films in order to evaluate the applicability of a Nd-YAG laser to low-temperature polycrystalline Si technology. The irradiation of a green laser was controlled during the crystallization of amorphous Si thin films deposited onto glass substrates in a sophisticated process. Raman spectroscopy and UV-Visible spectrophotometry were employed to quantify the degree of crystallization in the Si thin films in terms of its optical transmission and vibrational characteristics. The effectiveness of the Nd-YAG laser is suggested as a feasible alternative that is capable of crystallizing the amorphous Si thin films.