Much recent research has focused on the development lead-free perovskite piezoelectrics as environmentally compatible alternatives to lead zirconate titanate (PZT). Two main categories of lead free perovskite piezoelectric ceramic systems were investigated as potential replacements to lead zirconate titanate (PZT) for actuator devices. First, solid solutions based on Li, Ta, and Sb modified (K���.���Na���.���)NbO��� (KNN) lead-free perovskite systems were created using standard solid state methods. Secondly, Bi-based materials a variety of compositions were explored for (1-x)(Bi���.���Na���.���)TiO���-xBi(Zn���.���Ti���.���)O��� (BNT-BZT) and Bi(Zn���.���Ti���.���)O������(Bi���.���K���.���)TiO������(Bi���.���Na���.���)TiO��� (BZT-BKT-BNT). It was shown that when BNT-BKT is combined with increasing concentrations of Bi(Zn[subscript 1/2]Ti[subscript 1/2])O��� (BZT), a transition from normal ferroelectric behavior to a material with large electric field induced strains was observed. The higher BZT containing compositions are characterized by large hysteretic strains (> 0.3%) with no negative strains that might indicate domain switching. This work summarizes and analyzes the fatigue behavior of the new generation of Pb-free piezoelectric materials. In piezoelectric materials, fatigue is observed as a degradation in the electromechanical properties under the application of a bipolar or unipolar cyclic electrical load. In Pb-based materials such as lead zirconate titanate (PZT), fatigue has been studied in great depth for both bulk and thin film applications. In PZT, fatigue can result from microcracking or electrode effects (especially in thin films). Ultimately, however, it is electronic and ionic point defects that are the most influential mechanism. Therefore, this work also analyzes the fatigue characteristics of bulk polycrystalline ceramics of the modified-KNN and BNT-BKT-BZT compositions developed. The defect chemistry that underpins the fatigue behavior will be examined and the results will be compared to the existing body of work on PZT. It will be demonstrated that while some Pb-free materials show severe property degradation under cyclic loading, other materials such as BNT-BKT-BZT essentially exhibit fatigue-free piezoelectric properties with chemical doping or other modifications. Based on these results, these new Pb-free materials have great potential for use in piezoelectric applications requiring a large number of drive cycles such as MEMS devices or high frequency actuators. / Graduation date: 2013