Porous Ba0.67Sr0.33TiO3 (BST) ceramics were fabricated by the solid‐state reaction process, and their micro‐structural, dielectric, and pyroelectric properties were systemically investigated. Compared with dense specimens, porous BST exhibited a higher pyroelectric coefficient (p), a lower dielectric constant (ɛ), and heat capacity (CV), which are beneficial for the development of pyroelectric devices. At room temperature, as the porosity increased from 1.0% to 9.6%, BST ceramics' pyroelectric coefficient increased from 5000 to 8000 μc·(m2·°C)–1, the dielectric constant decreased from 12 000 to 8000, while the dielectric losses were <1.0% and the figure‐of‐merit
increased from 11.0 × 10−5 to 27.0 × 10−5Pa−0.5. Improvement of pyroelectric property is benecial for the development of infrared detectors.