PbZr0.4Ti0.6O3 (PZT) thin films with high crystallinity and high remanant polarization (Pr) have been fabricated by sol-gel deposition with pulsed excimer (XeCl) laser annealing at low process temperatures. The amorphous PZT films were prepared on Pt/Ti/SiO2/Si substrates by a sol-gel method. The deposited amorphous PZT films were annealed at 550 for 10 min. to initiate the nucleation of the PZT perovskite phase, and then annealed with an UV pulsed excimer laser (308 nm) heating at 400. X-ray diffraction (XRD) patterns show that 150-230 mJ/cm2 range multi-shot excimer laser irradiation drastically improved the crystallinity of the PZT perovskite phase. Field emission SEM (FE SEM) image show that the PZT thin film has uniform-sized crystal grains. The ferroelectric properties were found to depend on the laser energy density and shot number.