(Pb0.87−0.07xBa0.10+0.07x)La0.02(Zr0.7Sn0.15Ti0.15)O3 ceramics with 0 ≤ x ≤1 were prepared by conventional solid-state reaction process, and their dielectric and electric field–induced pyroelectric properties were systemically investigated. Compared with conventional pyroelectric materials, (Pb0.87−0.07xBa0.10+0.07x)La0.02(Zr0.7Sn0.15Ti0.15)O3 ceramics exhibited higher pyroelectric coefficient and figure of merit, which are beneficial for the development of pyroelectric devices. The specimens with x = 0.65 showed good pyroelectric properties for practical applications. When a 500 V/mm dc bias field was applied, they showed the maximum pyroelectric coefficient of 12,200 μC/m2K and the figure of merit of 106 × 10−5 Pa−0.5 at 45 °C, which are larger than those observed from conventional pyroelectric materials. Improvement of pyroelectric property is beneficial for the development of infrared detectors.