AbstractTransition metal oxides exhibit a plethora of electrical and magnetic properties described by their order parameters. In particular, ferroic orderings offer access to a rich spectrum of fundamental physics phenomena, in addition to a range of technological applications. The heterogeneous integration of ferroelectric and ferromagnetic materials is a fruitful way to design multiferroic oxides. The realization of freestanding heterogeneous membranes of multiferroic oxides is highly desirable. In this study, epitaxial BaTiO3/La0.7Sr0.3MnO3freestanding bilayer membranes are fabricated using pulsed laser epitaxy. The membrane displays ferroelectricity and ferromagnetism above room temperature accompanying the finite magnetoelectric coupling constant. This study reveals that a freestanding heterostructure can be used to manipulate the structural and emergent properties of the membrane. In the absence of the strain caused by the substrate, the change in orbital occupancy of the magnetic layer leads to the reorientation of the magnetic easy‐axis, that is, perpendicular magnetic anisotropy. These results of designing multiferroic oxide membranes open new avenues to integrate such flexible membranes for electronic applications.