Some dielectrics with ferroelectric, pyroelectric, and/or piezoelectric characteristics are widely used for medical ultrasound imaging and actuators, electro-optic modulators, optical display devices, nonvolatile memories, data storage, sensors, etc. [1] Among all the ferroelectrics known today, lead zirconate titanate (PZT) (PbZr 1-x Ti x O 3 )-based materials have a wonderful piezoelectric property and, thus, have been used for actuators, transducers, energy harvesters, etc. [1,2] The appearance of morphotropic phase boundary (MPB) at about 50% Zr-substitution for Ti 4þ at the B-site of ABO 3 perovskite structure makes the PZT materials more interesting. The MPB region connects tetragonal as well as rhombohedral phase appearing for the Ti-and Zr-rich compounds, respectively. [3] The MPB enhances the properties of the material and, thus, appears with the variation of the precursors and processing conditions of the systems. There are many lead-free piezo-materials, such as: BiNaTiO 3 , BaTiO 3 , KNaNbO 3 , and BiKTiO 3 , which has a small piezoelectric coefficient and figure of merit, and, thus, less capacity to tune the piezoelectricity as compared with that of PZT. Though there is a ban on the PZT-based materials to be used for devices due to their toxicity, PZT will be chosen till the availability of an alternate lead-free material having better piezoelectricity. A maximum (233 pC/N) piezoelectric property is found at the MPB of PZT with Zr/Ti¼52/48. [4] The piezo-coefficient d 33 value has been recorded as 471 pC/N for ZnO-substituted PZT. [5] In practice, PZT ceramics are frequently modified to meet the tough requirements for applications as well. However, a small dielectric loss under high fields and a maximum relative permittivity are desirable. In general, the substitution of different elements at the A-and/or the Bsites leads to get the modified and better piezoelectric property. To get an outstanding result, a number of ions including Naþ and Kþ at the A-site (Pb) and Fe 3þ , Fe 2þ , Co 3þ , Co 2þ , Mn 3þ , Mn 2þ , Mg 2þ , Ni 2þ , Al 3þ , In 3þ , Ga 3þ , Sc 3þ , and Cr 3þ ions at the B-site (Zr/Ti) of PZT ceramic are substituted. It has been seen that Zn ion substitution lowers loss tangent of a material. [6] Again, increasing ZnO content in PZT reduces the grain size and, thus, enhanced mechanical and piezoelectric property. [7] PZT along with Nb 2 O 5 gave optimum dielectric as well as piezoelectric properties. [8,9] ZnO in its nanoform has attracted much attention of scientists for its piezoelectric, optoelectronic, electrical, and microwave absorption properties for several decades. ZnO-embedded PZT showed better tunable electrical [10] and mechanical properties. Furthermore, the incorporation of ZnO lowered sintering temperature and improved the electrical property of the host material. [5] The crack-free double-scale lead zirconium titanate Pb(Zr 0.52 Ti 0.48 )O 3 (PZT52/48) with a Zr/Ti ratio of 52/48 has become a potential candidate for excellent electrical and mechanical properties for applicat...