Self‐folding films are a unique kind of thin film. They are able to deform in response to a change in environmental conditions or internal stress and form complex 3D structures. They are very promising candidates for the design of bioscaffolds, which resemble different kinds of biological tissues. In this paper, a very simple and cheap approach for the fabrication of fully biodegradable and biocompatible self‐rolled tubes is reported. The tubes' folding can be triggered by temperature. A bilayer approach is used, where one component is active and another one is passive. The passive one can be any biocompatible, biodegradable, hydrophobic polymer. Gelatin is used as an active component: it allows the design of (i) self‐folding polymer films, which fold at room temperature (22 °C) and irreversibly unfold at 37 °C, and (ii) films, which are unfolded at room temperature (22 °C), but irreversibly fold at 37 °C. The possibilities of encapsulation of neural stem cells are also demonstrated using self‐folded tubes.

We discovered a new and unexpected effect of reversible actuation of ultrathin semicrystalline polymer films. The principle was demonstrated on the example of thin polycaprolactone-gelatin bilayer films. These films are unfolded at room temperature, fold at temperature above polycaprolactone melting point, and unfold again at room temperature. The actuation is based on reversible switching of the structure of the hydrophobic polymer (polycaprolactone) upon melting and crystallization. We hypothesize that the origin of this unexpected behavior is the orientation of polycaprolactone chains parallel to the surface of the film, which is retained even after melting and crystallization of the polymer or the “crystallization memory effect”. In this way, the crystallization generates a directed force, which causes bending of the film. We used this effect for the design of new generation of fully biodegradable thermoresponsive polymeric actuators, which are highly desirable for bionano-technological applications such as reversible encapsulation of cells and design of swimmers.

A novel approach for fabrication of 3D cellular structures using new thermosensitive shape‐changing polymer films with photolithographically patterned surface—4D biofabrication is reported. The surface of shape‐changing polymer films is patterned to selectively adsorb cells in specific regions. The 2D cell pattern is converted to the 3D cell structure after temperature‐induced folding of the polymer films. This approach has a great potential in the field of tissue engineering and bioscaffolds fabrication.