In the present research, an approach of converting amorphous-silicon (a-Si) thin films into polycrystalline thin films using the third harmonics of an all-solid-state pulsed Nd 3+:YAG laser (355 nm) is studied. Two different samples of a-Si thin films on alkali-free glass (a-Si/glass) substrates and a-Si thin film on crystalline-Si substrates (a-Si/c-Si) are laser treated at different laser fluences ranging from 170 to 960 mJ/cm 2. The amount of heat incident on the surface has been analyzed theoretically by solving the one-dimensional heat-equation model. The ablation threshold, the region of crystallization and the depth of crystallization have been investigated theoretically. The influence of laser irradiation, ablation and crystallinity has been experimentally analyzed through in-situ reflectivity measurements, scanning electron microscopy (SEM) and Raman spectroscopy studies. In the case of a-Si/c-Si, the extent of crystallinity and the influence of structural characteristics on electronic properties are studied using the Hall-effect technique. The ablation threshold and the range of crystallization regime are in good agreement with the theoretical results. Laser fluence between 300 and 500 mJ/cm 2 is required for crystallization and the ablation threshold is estimated to be above 500 mJ/cm 2 for a-Si thin film with a thickness up to 400 nm.