ZnO-doped Li-0.06(Na0.535K0.48)(0.94)NbO3 ceramics were synthesized by a conventional mixed-oxide method. A dense microstructure was achieved and was free from deliquescence when ZnO was added. With adding 0.6 mol% ZnO, the Zn2+ first enters the A-site, while higher amounts of Zn2+ substitutes B-site ions. The addition of ZnO changes the ceramics to "hard'' performance with improvement of Q(m) to 235. A phase transition from tetragonal to orthorhombic phase was obtained in the compositional range of 0.6-0.8 mol% ZnO. Because of such transitional behavior, d(33), k(p), and epsilon(r) reached peak values of 250 pC/N, 45%, and 986, respectively. Crown Copyright (C) 2010 Published by Elsevier B.V. All rights reserved.