Li, Ta modified (K,Na)NbO3 single crystals with the size of 18 mm × 18 mm × 10 mm were successfully grown by top-seeded solution growth method, with orthorhombic-tetragonal phase transition temperature ~79 °C and Curie temperature ~276 °C. The electromechanical coupling factors k33 and kt were found to be ~88% and ~65%, respectively. The piezoelectric coefficient d33 for the [001]c poled crystals reached 255 pC/N. In addition, the electromechanical coupling factor exhibited high stability over the temperature range of -50 °C to 70 °C, making these lead free crystals good candidates for electromechanical applications.