We report excellent electrostrain properties of (1 − x)BaTiO3–xSrSnO3 (BSTS) Pb‐free electroceramics (0 ≤ x ≤ 0.15), as well as the corresponding structural, dielectric, and ferroelectric properties. A tailored phase diagram of the pseudo‐binary solid solution of BaTiO3–SrSnO3, which exhibits a nearly composition‐independent orthorhombic–tetragonal polymorphic phase boundary close to room temperature, was obtained, and, in contrast to Ba(Ti1−xSnx)O3, the appearance of the relaxor mode was accelerated in the phase transition of BSTS owing to the additional incorporation of Sr. Using these compositionally modified phase‐related characteristics, desirable sets of electrostrain properties for actuator applications were obtained. Based on these results, we propose that BSTS is a promising candidate for Pb‐free electroceramics for high‐precision actuator applications near room temperature.