In Ba0.6Sr0.4TiO3 (BSTO)‐based epitaxial nanocomposite films increased P
r values are demonstrated by up to a factor of 3 compared to standard BSTO films. A strongly reduced temperature coefficient of polarization retention is also obtained, i.e., 0.07% °C−1 compared to 0.24% °C−1. Piezopoling with only marginal leakage current is also achieved up to 200 °C, the highest temperature studied. The origin of the improved performance is the incorporation of Sm2O3 nanopillars in the films which acted as stiff vertical nanoscaffolds, inducing a strong tetragonal distortion in the BSTO (up to 1.033(7) in terms of the out‐of‐plane/in‐plane lattice dimensions). The films have comparable performance to industry‐standard Pb(Zr,Ti)O3 films, at the same time as being Pb‐free.