In this work, we report the electromechanical properties of 〈00l〉C-textured (K0.5Na0.5)0.98Li0.02NbO3 (KNLN) and (K0.5Na0.5)(Nb0.85Ta0.15)O3 (KNNT) ceramics produced by templated grain growth. Both materials show high texture quality (F00l=98% and full-width at half-maximum [FWHM]=8.4° for KNLN, F00l=99%, and FWHM=7.6° for KNNT) and enhanced piezoelectric response compared with randomly oriented ceramics. However, textured KNLN shows higher piezoelectric properties (d33=192 pC/N, kp=0.63, k31=0.39, d31=−73 pC/N, d33*=208 pC/N) and higher phase transition temperatures (To−t=155°C, Tc=439°C) than textured KNNT. The enhanced room-temperature piezoelectric properties are associated with low-strain hysteresis (4.0%), suggesting that 〈00l〉C textured and poled orthorhombic KNLN may exhibit domain engineering character. The piezoelectric performance of textured KNLN with To−t=155°C is high and stable over a wide temperature range (−60°–100°C), strongly favoring use of this material in device applications compared with the modified KNN-based materials with a To−t near room temperature.