Ferroelectric nanotubes offer intriguing opportunities for stabilizing exotic polarization domains and achieving new or enhanced functionalities by tailoring the complex interplay among the geometry, surface effects, crystal symmetry, and more. Here, phase‐field simulations to predict the room‐temperature equilibrium polarization domain structure in (001)pc PbZr0.52Ti0.48O3 (PZT) nanotubes are used (pseudocubic (pc)). The simulations incorporate the influence of surface‐tension‐induced strains, which have been ignored in existing computational studies. It is found that (001)pc PZT nanotubes can host a unique class of topological polarization domain structures comprising non‐planar flux‐closures and anti‐flux‐closures that are inaccessible with ferroelectrics of planar geometry (e.g., thin‐films, nanodots). It is shown that surface‐tension‐induced strain is significantly enhanced in thin‐walled nanotubes and thereby can lead to noticeable modulation of the flux closures. Domain stability map as a function of the nanotube wall thickness and height is established. The results provide a basis for geometrical engineering of domain structures and associated functional (e.g., piezoelectric, electrocaloric) responses in ferroelectric nanotubes.

Interlayer coupling in materials, such as exchange interactions at the interface between an antiferromagnet and a ferromagnet, can produce exotic phenomena not present in the parent materials. While such interfacial coupling in magnetic systems is widely studied, there is considerably less work on analogous electric counterparts (i.e., akin to electric “exchange‐bias‐like” or “exchange‐spring‐like” interactions between two polar materials) despite the likelihood that such effects can also engender new features associated with anisotropic electric dipole alignment. Here, electric analogs of such exchange interactions are reported, and their physical origins are explained for bilayers of in‐plane polarized Pb1−xSrxTiO3 ferroelectrics. Variation of the strontium content and thickness of the layers provides for deterministic control over the switching properties of the bilayer system resulting in phenomena analogous to an exchange‐spring interaction and, leveraging added control of these interactions with an electric field, the ability to realize multistate‐memory function. Such observations not only hold technological promise for ferroelectrics and multiferroics but also extend the similarities between ferromagnetic and ferroelectric materials to include the manifestation of exchange‐interaction‐like phenomena.