Textured PMN-PZT fabricated by templated grain growth (TGG) method has a piezoelectric coefficient (d) of 3 to 5 times that of its random counterpart. By combining this TGG method with low-temperature co-firing ceramics (LTCC) techniques, co-fired multilayer textured piezoelectric ceramic materials with inner electrodes were produced at a temperature as low as 925° C., which silver could be used. Trilayer PMN-PZT ceramics prepared by this method show a strain increase of 2.5 times, a driving voltage decrease of 3 times, and an equivalent piezoelectric coefficient (d*) improvement of 10 to 15 times that of conventional random ceramic counterparts. Further, a co-fired magnetostrictive/piezoelectric/magnetostrictive laminate structure with silver inner electrode was also synthesized. The integration of textured piezoelectric microstructure with the cost-effective low-temperature co-fired layered structure achieves strong magnetoelectric coupling. These new materials have promising applications including as actuators, ultrasonic transducers, and use in energy harvesters.