Excimer laser crystallization is used to produce layered nanocrystalline silicon from hydrogenated amorphous silicon, using a partial melting process. Three types of hydrogenated amorphous silicon samples, 100, 300, and 500 nm thick, were laser treated in order to investigate the changes to the structural, optical, and electrical properties as a function of amorphous silicon thickness with excimer laser crystallization. The resulting nanocrystalline thin films were characterized using Raman spectroscopy, optical absorption measurements, atomic force microscopy, forward recoil spectrometry, and current-voltage measurements. The relationship of crystalline volume and laser energy density was established, along with the behavior of the optical gap and its relationship to hydrogen content. Surface roughness effects are discussed in the context of photovoltaic applications. The effect of increased mobility on photoconductivity after excimer laser crystallization is also examined.