F erroelectric materials exhibit multifunctional properties such as piezoelectricity, nonvolatile charge, and electrooptic functions. 1−5 Accordingly, ferroelectric materials have been an interesting subject of intensive scientific investigation, especially for ferroelectric nonvolatile random access memories (FeRAM) and actuators. 5−10 Basically, ferroelectric memories utilize the remanent polarization originating from the employed ferroelectric materials themselves, enabling suitable operation by charge detection. 11,12 Once electric polarization is changed by an external electric field, piezoelectric strain is generated under the biased states. 13,14 Even though the applied electric field is switched off, two different polarized states still remain to be observed and thereby can be utilized for nonvolatile digital information. In contrast, piezoelectric strains cannot possess these nonvolatile characteristics with the two observable different states because the generated piezoelectric strains are returned to the same positions without an applied electric field. 5 In other words, a symmetric piezoelectric butterfly curve is expected with regard to the piezoelectric strain axis, indicating that no shape memory window is available.Meanwhile, an imprint, which is a defect (e.g., fatigue) in a ferroelectric material, is known to generate a shift in the ferroelectric hysteresis loop, leading to a failure of stored ferroelectric information. 15 Therefore, the symmetric piezoelectric butterfly curve can be shifted to be asymmetric in piezoelectric thin films by virtue of an electrical imprint field. 16−18 It is interesting to note that the shifted hysteresis loop with an asymmetric piezoelectric strain provides a potential operating source for nonvolatile piezoelectric shape memory. 5 The origin of this imprint effect in ferroelectric materials is the internal electric field induced by electrode configurations, trapped charge, and external processes such as optical and thermal processes. 18−22 In terms of realizing the use of piezoelectric strains in ferroelectric materials, Morita et al. demonstrated that control of the imprint electric field, which is induced by treatment with a high electrical field of 3.5 kV/mm at 150°C, could be used to produce viable piezoelectric shape memory devices. 5 Motivated by these intriguing possibilities in innovative memory applications, we believe that the artificial manipulation of imprint effects is essential to achieve highly efficient nonvolatile shape memories. 23 Herein, we propose that the ferroelectric multilayer structure composed of two different ferroelectric thin films enables artificial control of the imprint effect in ferroelectric hysteresis. More specifically, we show that the shift in ferroelectric hysteresis could be effectively modulated by adjusting the thickness of each ferroelectric layer or the thickness ratio in the ferroelectric multilayered schemes. On the basis of a theoretical firstprinciples calculation, we estimated characteristics of the depolarization...