AbstractMn‐doped 0.36Pb(In1/2Nb1/2)O3–0.36Pb(Mg1/3Nb2/3)O3–0.28PbTiO3 [Mn‐PIMNT(36/36/28)] thin films were fabricated by pulsed laser deposition. The microstructures and ferroelectric, piezoelectric, dielectric, pyroelectric properties were investigated. The films exhibited a (111) orientation as well as a uniform and dense surface. The Raman spectra revealed that the films showed a rhombohedral phase at room temperature, rhombohedral to tetragonal, and tetragonal to paraelectric phase transitions near 150℃ and 250℃, respectively. Furthermore, the films exhibited a high remnant polarization (Pr) of 51.3 μC cm−2, a coercive field (EC) of 3.14 kV mm−1, a high normalized piezoelectric strain coefficient () up to 47 pm V−1, a pyroelectric coefficient (p) up to 8.5 × 10−4 C m−2 K−1, and dielectric constant (εr) of 2824, as well as excellent dielectric tunability of 89% at room temperature. The excellent ferroelectric and pyroelectric properties combined with high Curie point indicate that the Mn‐PIMNT(36/36/28) films are a potential candidate for ferroelectric and pyroelectric devices.