toward flexible sensors, [4] actuators, [5] memory cells, [6] and circuits [7] in the last decade, such functionalities are largely accomplished at the system level relying on flexible substrate, and intrinsically flexible multifunctional materials remain rare except in organic forms. For inorganic materials such as functional oxides that often require high temperature processing incompatible with polymeric substrates, [8,9] this imposes a serious obstacle. One such example is multiferroics with simultaneous electric and magnetic orderings, [10] which are highly desirable for sensing, actuation, data storage, as well bio-inspired systems, [11][12][13][14] yet developing flexible materials with robust multiferroic properties at room temperature is a longterm challenge. Flexible multiferroics have been reported on polymer substrates [15] or in polyvinylidene fluoride based nanocomposites, [16,17] but they are restricted by their low tolerance to high temperature processing as well as operations, and their performances are usually inferior to inorganic systems. Oxide multiferroics on metal foils [18] or mica substrate [19,20] have also been reported, though they are restricted by the substrates with low stretchability, and their flexibility is limited as well.Multiferroics with simultaneous electric and magnetic orderings are highly desirable for sensing, actuation, data storage, and bio-inspired systems, yet developing flexible materials with robust multiferroic properties at room temperature is a long-term challenge. Utilizing water-soluble Sr 3 Al 2 O 6 as a sacrificial layer, the authors have successfully self-assembled a freestanding BaTiO 3 -CoFe 2 O 4 heteroepitaxial nanostructure via pulse laser deposition, and confirmed its epitaxial growth in both out-of-plane and in-plane directions, with highly ordered CoFe 2 O 4 nanopillars embedded in a single crystalline BaTiO 3 matrix free of substrate constraint. The freestanding nanostructure enjoys super flexibility and mechanical integrity, not only capable of spontaneously curving into a roll, but can also be bent with a radius as small as 4.23 µm. Moreover, piezoelectricity and ferromagnetism are demonstrated at both microscopic and macroscopic scales, confirming its robust multiferroicity at room temperature. This work establishes an effective route for flexible multiferroic materials, which have the potential for various practical applications.