Stress-free two-way shape memory polymers capable of reversible shifting between two distinct shapes offer versatile platforms for the development of future smart devices. However, improving the recovery performance of bidirectional shape memory polymers with good biocompatibility and stimulus temperature remains challenging. Studies have shown that enhancing oriented crystallization can effectively improve shape recovery performance. Herein, we demonstrate a simple approach to enhance the number of nanofibers aligned in the tensile stress direction by controlling the alignment direction of polycaprolactone nanofibers, which promotes the generation of oriented crystallization in the tensile state, thereby achieving a 230.8% improvement in recoverable strain. The optimization of the nanofiber structure offers a generalized method for enhancing the two-way shape memory behavior of semicrystalline polymers.
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