Self-separated Pb(Zr(0.52)Ti(0.48))O(3) (PZT) films were processed by a hydrothermal deposition and a rapid thermal separation method, followed by a sol-gel filling and sintering process. The films possess excellent piezoelectric and electromechanical properties close to those of bulk material. The maximum remnant polarization is over 30 μC/cm(2) and the electromechanical coupling factor (k(t)) reaches as high as 0.52. The unique microstructure characteristics of the PZT films, such as their highly dense structure, columnar grains, well-connected grain boundaries, and well-dispersed nanopores, could all contribute to the enhanced piezoelectric and electromechanical properties.