Piezoelectrics are key materials for energy conversion, for example in ultrasound transducers and energy harvesters. This work presents the synthesis and characterization of the lead-free piezoelectric composition (Li0.06(K0.52Na0.48)0.94)(Nb0.71Ta0.29)O3 doped with 0.25 mol% Mn (KNNLTM) as textured ceramics. Templated grain growth from NaNbO3 platelet templates aligned by tape casting was used to introduce texture, and after sintering for 14 h at 1100 °C this produced up to 84% (100)pc grain orientation. After high temperature poling, the textured samples exhibit reasonable piezoelectric response with d
33 values up to 171 pC N−1, and k
t values of 0.35, which is 71% of the response obtained in a single crystal of the same composition. The low relative dielectric permittivity of the textured and high temperature-poled KNNLTM (ϵ
33
T/ϵ
0 down to 182) resulted in record-high piezoelectric voltage constants (g
33 up to 101 mV m N−1), higher than previously reported for lead-free piezoelectric ceramics, as well as very high figure of merit (d
33
g
33 up to 16 × 10−12 m3 J−1) for non-resonant energy harvesting in compression. These numbers make the textured KNNLTM materials of this work highly promising for use in thickness mode, non-resonant piezoelectric energy harvesters.