Nacre-Inspired Polymeric Materials with Body Heat-Responsive Shape-Memory Effect, High Optical Transparence, and Balanced Mechanical Properties

In this work, inspired by the hierarchical architecture of nacre, we have fabricated poly(propylene carbonate) (PPC)/thermoplastic polyurethane (TPU) alternating multilayer films via layer-multiplying coextrusion. Based on the glass transition at around 37 °C of PPC, the multilayer films exhibited an outstanding body heat-responsive shape-memory effect (SME) with high shape fixation and recovery ratios (96.1 and 93.6%), much better than the conventional cocontinuous blend with the same compositions. It was revealed that the high phase continuity and abundantly two-dimensional interfaces both capable of promoting stress transferring and load distribution maximally contributed to the SME. Furthermore, the multilayer films showed a superior recovery stress storage capacity and the force generated by shape recovery allowed automatic expansion of the spiral in 37 °C water and efficient lifting of a load 880 times its weight. Different from the opacity of the blend, a high optical transparence was observed in the multilayers because of the parallel assembly of transparent PPC and TPU enabling light to directly pass through the films. Besides, the nacre-like films had layer debonding and layer stepwise breaking during stretching, resulting in a 90% increase in tensile strength, a 70% increase in elongation at break, and onefold improvement in yield stress, compared with those of the blend. Our approach paves a new way for developing bioinspired structural materials with excellent optical, mechanical, and shape-memory properties, which can be extended to different amorphous polymers and elastomers. Also, the materials presented herein have great potential in applications of biomedical devices and soft robotics.