Lead lanthanum zirconium titanate (PLZT) ceramics belong to the family of materials known as smart materials, which can be used as sensors and actuators; however, the high dielectric, ferroelectric (P r ), and piezoelectric (d 33 and g 33 ) properties decide the end applications. The d 33 is related to charge generation or electric field-induced strain in the materials. On the other hand, g 33 and k p are related to the voltage generation and conversion of mechanical stress to the electric charge, respectively. High values of d 33 , g 33 , and k p are good for energy harvesting applications; however, the high-strain materials are more useful for actuators. The remanent polarization (P r ) and coercive field (E c ) are taken into cognizance for memory and energy density applications. High dielectric constant materials can be used for charge storage applications. (Pb 0.92 La 0.08 )(Zr 0.60 Ti 0.40 ) O 3 (PLZT 8/60/40) ceramics are known to show all of the above electrical properties. Further improvement of these properties is possible by modified processing approaches. In this study, it was found that a combination of mechanical activation (high-energy milling or HEM) with a cold isostatic process (CIP) not only reduces the processing temperatures and time but also circumvents the need to add any excess PbO in the starting materials. At the same time, the high density of ceramics was not compromised. No binder was added in this process, thereby avoiding the contamination risk involved and also the possibility of reduced density. Apart from the above two processes, yet another process that was used to improve the electrical properties output was a scientific study of the electrical poling process. The optimized poling results in the significant enhancement of electrical properties, which successfully increased piezoelectric properties multiple times. The PLZT 8/60/40 ceramics were effectively poled at fields less than the coercive field (<0.5E c ), which could be very advantageous especially in the case of ceramics have poor resistivity. Such PLZT ceramics is used for different types of defense applications.