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Due to environmental concerns and the increasing drive towards miniaturization of electronic circuits and devices, lead-free ferroelectric films with low leakage current and robust ferroelectric and piezoelectric properties are highly desired. The preferred alternative, BaTiO 3 , is non-toxic and has ferroelectric properties, but its high leakage current, poor ferroelectricity and piezoelectricity and low Curie temperature of ∼130 °C in thin film form are obstacles for high-temperature practical applications. Here, we report that a negative-pressure-driven enhancement of ferroelectric Curie temperature and effective piezoelectric coefficient are achieved in (111)-oriented BaTiO 3 nanocomposite films. The enhanced ferroelectric and piezoelectric properties in the emergent monoclinic BaTiO 3 are attributed to the sharp vertical interface and 3D tensile strain that develops upon interspersing stiff and self-assembled vertical Sm 2 O 3 nanopillars through the film thickness. Our work also demonstrates that fabricating oxide films through (111)-oriented epitaxy opens up new avenues for the creation of new phase components and exploration of novel functionalities for developing oxide quantum electronic devices.