Shape memory polymers (SMPs), as a class of intelligent materials, have shown great potential in biomedical and robotic fields. Although efforts have been made to design and fabricate SMPs in the past decades, most of the SMPs are not suitable for use in the human body due to their unpleasant triggering conditions. Furthermore, it is of great importance to diversify the shape memory effect (SME) of SMPs to extend their applications. In this work, through thiol-ene chemistry, SMPs based on random cross-linked hydrophobic polytetrahydrofuran (PTHF) and hydrophilic poly­(ethylene glycol) (PEG) oligomers were facilely fabricated. These SMPs showed a body temperature-triggered two-way SME with a reversible strain of up to 25.2%. Besides, the SMPs exhibited a good body temperature- and water-triggered one-way triple-SME. These features bestowed the polymers with a bright future in biomedical applications. Polymer P60-G40 was applied as a new type of esophageal stent, and the in vitro assessment showed that the stent was adjustable, self-expandable, and had the ability to release drugs, which were attributed to the one-way triple-SME and two-way SME.

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Shape memory polymers (SMPs) with the permanent shape reconfiguration capability have received much research interest because they are capable of diversified tasks and the ability to work in conditions that required complex geometry. However, most of such SMPs are thermally triggered, which limits their applications. Inspired by reversible mussel adhesive protein chemistry, NIR light‐triggered SMPs with the permanent shape reconfiguration capability are prepared. The polymer networks are constructed using biocompatible polyethylene glycol, which is crosslinked based on catechol–Fe3+ coordination. The polymer networks have a uniform network structure and exhibit a considerable one‐way shape memory effect (1W‐SME) as well as a good two‐way shape memory effect (2W‐SME) under stress conditions. Taking advantage of the dynamic nature of the catechol–Fe3+ coordination, the permanent shape of the polymers could be reconfigured. Moreover, the catechol–Fe3+ complexes have a broad absorption in the NIR window, which bestows the polymers with excellent NIR light‐triggered SME. Further, the great potential of the obtained polymers in biomedical and electronic applications is presented. Owing to the NIR‐triggered 1W‐SME and the permanent shape reconfiguration capability, the polymer could be used as a personalizing vascular stent. Additionally, the polymer could be applied in light‐driven switches based on the NIR light‐triggered 2W‐SME.