The toxicity and volatility of lead oxide, a main component utilized in the commercial production of lead-based piezoelectric ceramics, are the critically environmental issues that cannot be overlooked. Currently, European Union (EU) has issued the directives on waste of electrical and electronic equipments (WEEE) and restriction on the uses of hazardous substances (RoHS) which will be effective in the near future. Although PbO in lead-based piezoelectric ceramics are still an exception of the obligation since no material possesses piezoelectric properties superior to them, the need for lead-free piezoelectric compositions is still of commercial importance. The templated grain growth technique is of interest due to the possibility to achieve textured ceramics for large-scale production. The properties of seeds, polycrystalline matrix and fabrication technique are the critical key factors for successful grain orientation piezoelectric ceramics. The single-crystal seeds should possess anisotropic morphology, desired crystallographic orientation and lattice parameters similar to the crystals to be grown from the matrix. Meanwhile, the polycrystalline matrix should have very fine particles sufficient to accelerate a driving force in crystal growth and densification during sintering. Various perovskite components, i.e., BaTiO3, SrTiO3 and PbTiO3, were introduced as the seed compositions. Several techniques, i.e., molten salt, sol-gel, precipitation, reactive sintering, modified mixed-oxide, and mechanochemical methods, have been used to synthesize very fine particles for the polycrystalline matrix. In this work, the research collaboration between Rutgers, the State University of New Jersey, and MTEC, Piezoelectric sub-program, will be established to develop lead-free piezoelectric system. The bismuth sodium titanate (BNT) and bismuth titanate (BiT) based single crystals are prepared to act as seeds for TGG while the BNT-based powders are synthesized via modified mixed-oxide routes. The attrition and/or jet milling are applied to produce very fine particles after calcination. Aqueous suspensions for tape-casting are chosen to fabricate the ceramic sheets. Reliable, economical expense and mass production route are expected to result in this work.