High electromechanical strains have been developed in this study in Barium Titanate ceramics, suitably doped with Nd and Zr to form a controlled concentration gradient, leading to a dome-like structure on sintering. Compacted pellets constituted of layers of barium titanate powder of varying minor amounts of Nd and Zr powders, incorporated as nitrates precursors, acquire this dome shape on sintering at 1300-1320 o C and cooling to the ambient temperature, the result of the residual thermoelastic strain. The dome structures exhibit high electromechanical responses, and the piezoelectric coefficients (deduced from electric field induced strains measurements in dome-up and dome-down positions) are also found to be exceptionally high. These Nd and Zr doped barium titanate structures could find applications as an environmentally benign material for fabrication of high displacement functionally graded electromechanical actuators in a single sintering step process.