Interfaces between materials present unique opportunities for the discovery of intriguing quantum phenomena. Here, we explore the possibility that, in the case of superlattices, if one of the layers is made ultrathin, unexpected properties can be induced between the two bracketing interfaces. We pursue this objective by combining advanced growth and characterization techniques with theoretical calculations. Using prototype La 2/3 Sr 1/3 MnO 3 (LSMO)/ BaTiO 3 (BTO) superlattices, we observe a structural evolution in the LSMO layers as a function of thickness. Atomic-resolution EM and spectroscopy reveal an unusual polar structure phase in ultrathin LSMO at a critical thickness caused by interfacing with the adjacent BTO layers, which is confirmed by first principles calculations. Most important is the fact that this polar phase is accompanied by reemergent ferromagnetism, making this system a potential candidate for ultrathin ferroelectrics with ferromagnetic ordering. Monte Carlo simulations illustrate the important role of spin-lattice coupling in LSMO. These results open up a conceptually intriguing recipe for developing functional ultrathin materials via interface-induced spin-lattice coupling.spin-lattice coupling | interfaces | magnetic/electric | structural transition | ultrathin films I nterface physics has emerged as one of the most popular methods to discover unique phenomena caused by broken symmetry (1-6). In transition metal oxide (TMO) interfaces, the different electronic, magnetic, lattice, and orbital properties of two adjoined materials lead to fascinating properties that are often radically different from those of the two component bulk materials (7-10). It would seem that we are on the verge of being able to design (11) or engineer (12) the properties of interfaces.Although the behavior of individual interfaces has been widely investigated, how two or more interfaces behave within superlattices (SLs) remains an interesting and open topic (13,14). As shown in Fig. 1A, when two interfaces are geometrically close enough, they can drastically alter the properties of the material in between because of proximity effects. Unlike layered compounds, such as Fe-based superconductors and cuprates, which have pronounced 2D properties, most perovskites with the chemical formula ABO 3 exhibit drastic decreases in their functionalities under reduced dimensionality (i.e., ultrathin materials). This property has hindered the exploration and development of active low-dimensional materials (15, 16). Therefore, exploring ultrathin materials confined by two interfaces is a rational approach to see whether interfacial effects can be exploited to achieve desired functionalities.In this work, we present an example of using the structural phase change induced by two adjacent interfaces as a route to design ultrathin TMOs. We choose two materials with distinct properties: BaTiO 3 (BTO), which in its bulk form, is polar ferroelectric, and La 2/3 Sr 1/3 MnO 3 (LSMO), which in its bulk form, is nonpolar/tilt ferromagnetic....