<p>Bismuth-layered structure piezoelectric ceramics have been successfully applied to high-temperature sensors and ferroelectric memories due to their high Curie temperature and special piezoelectric properties. However, their very low piezoelectric constants and high-temperature leakage currents have limited their popularization in applications. In this paper, (1-<i>x</i>) SrBi₄Ti₄O₁₅-<i>x</i>Bi₄Ti₃O₁₂ (<i>x</i> = 0, 0.2, 0.4, 0.6, 0.8, 1), bismuth-layered piezoelectric ceramics with an intergrowth structure are prepared by the high-temperature solid-phase method. The interactions among the intergrowth structure, concentration of oxygen vacancies, microstructure, and electrical properties of the BLSFs samples are investigated. The results of the scanning electron microscope (SEM) and X-ray photoelectron spectroscopy (XPS) should indicate that the grain size of the intergrowth is smaller than that of the non-intergrowth structure. The grain size decreases with the increase in oxygen vacancy energy for the samples with an intergrowth structure. The construction of the intergrowth structure has less effect on the dielectric loss. In addition, the construction of the intergrowth structure helps enhance piezoelectric performance overall. Among all the samples, the 0.6SrBi₄Ti₄O₁₅-0.4Bi₄Ti₃O₁₂ sample shows the best performance with a piezoelectric constant (<i>d</i>₃₃) of 21 pc/N, a Curie temperature (<i>T</i>_C) as high as 544&#xa0;°C, a dielectric loss (tan<i>δ</i>) of 0.9%, a relative dielectric constant (<i>ε</i>_r) of 164, and the lowest conductivity. It is shown that it has potential applications in the high-temperature field.</p>