In this letter the authors report the observation of double hysteresis loops in Cu-doped K0.5Na0.5NbO3 (KNN) ceramics. Unlike other ferroelectric titanates (e.g., BaTiO3), aging is not required for the ceramic to exhibit the double-loop-like characteristics. Based on the symmetry-conforming principle of point defects, it is suggested that defect dipoles are formed by the acceptor dopant ions-Cu2+ and O2− vacancies along the polarization direction after the diffuse tetragonal-orthorhombic phase transition of the ceramic. Because of the low migration rates of defects, the defect dipoles remain in the original orientation during the P-E loop measurement, providing a restoring force to reverse the switched polarization. The defect dipoles also provide “pinning” effects in the normal piezoelectric activities. As a result, the ceramic becomes “hardened,” exhibiting an extraordinarily high mechanical quality factor (2500), while the other piezoelectric properties remain reasonably good: electromechanical coupling coefficients kp = 39%, kt = 47%, and piezoelectric coefficient d33 = 82 pC/N.