A complete analysis of the morphology, crystallographic orientation, and resulting electrical properties of Pb(Zr0.53,Ti0.47) Pb(Nb1/3, Zn2/3)O3 (PZT-PZN) thin films, as well as the electrical behavior when integrated in a cantilever for energy harvesting applications, is presented. The PZT-PZN films were deposited using sol-gel methods. We report that using 20% excess Pb, a nucleation layer of PbTiO3 (PT), and a fast ramp rate provides large grains, as well as denser films. The PZT-PZN is deposited on a stack of TiO2/PECVD SiO2/Si3N4/thermal SiO2/Poly-Si/Si. This stack is designed to allow wet-etching the poly-Si layer to release the cantilever structures. It was also found that the introduction of the poly-Si layer results in larger grains in the PZT-PZN film. PZT-PZN films with a dielectric constant of 3200 and maximum polarization of 30 μC/cm2 were obtained. The fabricated cantilever devices produced ~300–400 mV peak-to-peak depending on the cantilever design. Experimental results are compared with simulations.