The ferroelectric properties of lead zirconate titanate (PZT) films crystallized by a continuous-wave (CW) green laser are discussed in this paper. After CW green laser annealing, two kinds of typical crystallization modes of the PZT thin films were observed: island crystallization and lateral crystallization. In the island crystallization region, the PZT film was crystallized uniformly over the thin films. However, poor surface roughness was found in lateral crystallization region. Significant improvements of ferroelectric characteristics have been achieved in the island crystallization region after optimizing with a low energy density. By varying energy density from 4.5 to 7.1 kW/cm2 and fixing annealing time at 42.5 ms, significant features were found at an energy density of 5.3 kW/cm2. A maximum remanent polarization of 27 µC/cm2 was obtained.