It is commonly assumed that the substantial element of reversibly actuating soft polymeric materials is chemical cross-linking, which is needed to provide elasticity required for the reversible actuation. On the example of melt spun and three-dimensional printed Janus fibers, we demonstrate here for the first time that cross-linking is not an obligatory prerequisite for reversible actuation of solid entangled polymers, since the entanglement network itself can build elasticity during crystallization. Indeed, we show that not-cross-linked polymers, which typically demonstrate plastic deformation in melt, possess enough elastic behavior to actuate reversibly. The Janus polymeric structure bends because of contraction of the polymer and due to entanglements and formation of nanocrystallites upon cooling. Actuation upon melting is simply due to relaxation of the stressed nonfusible component. This approach opens perspectives for design of solid active materials and actuator for robotics, biotechnology, and smart textile applications. The great advantage of our principle is that it allows design of non-cross-linked self-moving materials, which are able to actuate in both water and air, which are not cross-linked. We demonstrate application of actuating fibers for design of walkers, structures with switchable length, width, and thickness, which can be used for smart textile applications.
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