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All-oxide free-standing cantilevers were fabricated with epitaxial (001)-oriented Pb(Zr0.52Ti0.48)O3 (PZT) and Pb(Zr0.52Ti0.48)0.99Nb0.01O3 (PNZT) as piezoelectric layers and SrRuO3 electrodes. The ferroelectric and piezoelectric hysteresis loops were measured. From the zero-bias values, the figure-of-merits (FOMs) for piezoelectric energy harvesting systems were calculated. For the PNZT cantilever, an extremely large value FOM = 55 GPa was obtained. This very high value is due to the large shifts of the hysteresis loops such that the zero-bias piezoelectric coefficient e31f is maximum and the zero-bias dielectric constant is strongly reduced compared to the value in the undoped PZT device. The results show that by engineering the self-bias field the energy-harvesting properties of piezoelectric systems can be increased significantly.