Relaxor‐PbTiO3‐based ternary ferroelectric solid‐solution ceramics with high Curie temperature end members are effective to achieve broader usage temperature range and drive field stability, meanwhile with comparable piezoelectric responses to binary Pb(Mg1/3Nb2/3)O3‐PbTiO3 (PMN‐PT). Templated grain growth is viable alternative to crystal growth that uses templates to induce crystal orientation along a specific direction, thus enhancing the piezoelectric response. In this research, perovskite Pb(Sc1/2Nb1/2)O3‐PbZrO3‐PbTiO3 (PSN‐PZ‐PT) system with varying components is developed to determine the morphotropic phase boundary; together with the texturing characteristics, a high piezoelectric response with broad temperature usage range is expected. 37.5PSN‐20PZ‐42.5PT exhibits enhanced piezoelectric d33 of 530 pC N−1 and strain level of 0.20% at 20 kV cm−1, while retaining a high Curie temperature of 309 °C. Of particular interest is that a high piezoelectric voltage coefficient g33, totaling 56 × 10−3 Vm N−1 can be achieved in this composition, leading to a high figure of merit, (d33 × g33)/tan δ, of 5.8 × 10−10 m2 N−1, one order higher than that of PMN‐PT textured counterpart, being potential for energy harvesting and hydrophone applications.