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Abstract: A shift of the morphotropic phase boundary (MPB) and a superior piezoelectric response are observed in Nb-doped Pb(Zr x Ti1− x )O3 (PNZT) thin films epitaxially grown on Nb-doped SrTiO3(100) (Nb:STO) substrates. X-ray diffraction and Raman spectra characterizations confirm that a phase transition from a tetragonal structure to a rhombohedral structure occurs when the Zr/Ti ratio varies from 20/80 to 80/20. The phenomenological theory and experimental analyses suggest that the MPB of epitaxial PNZT thin films is shifted to the higher Zr/Ti ratio (around 70/30) from the conventional ratio (52/48) due to the misfit compressive stress induced by the substrate. A maximum local effective longitudinal piezoelectric coefficient (d 33) up to 307pmV−1 is observed at a Zr/Ti ratio of 70/30 in the current compositional range, again confirming the shifting of MPB in epitaxial PNZT thin films. These findings offer a new insight for the fabrication of epitaxial PZT thin films at MPB with a superior piezoelectric response. [Copyright &y& Elsevier]