Shape memory polymers (SMPs) show promise in areas like wearable electronics and soft robotics but often have low (actuation) energy densities (<1 MJ/m³), limiting their maximum load. Recent work suggests that periodically incorporating directional H-bonds can enable high-energy-density SMPs by forming stable strain-induced supramolecular nanostructures. Here, we found that adding weaker H-bonding units to the polymer can tune its actuation temperature from 60°C to 25°C while maintaining ∼80% of the energy density of the original polymer and achieving self-healing at accessible temperatures (∼70°C). By using this self-healable, high-energy SMP, we realized rapid healing of macroscopic film damage (e.g., centimeter-sized knife punctures) that was not healable in polymers without high-energy shape-memory-assisted self-healing (SMASH) behavior. The self-healing SMP was used to fabricate a self-healable force sensor with high cyclability and sensitivity, marking a significant advancement in creating tunable and self-healable SMPs for smart, durable wearable devices.

形状记忆聚合物 (SMP) 在可穿戴电子产品和软机器人等领域显示出前景，但通常具有较低的（驱动）能量密度（<1 MJ/m ³ ），限制了其最大负载。最近的研究表明，周期性结合定向氢键可以通过形成稳定的应变诱导超分子纳米结构来实现高能量密度的形状记忆聚合物。在这里，我们发现向聚合物中添加较弱的氢键单元可以将其驱动温度从 60°C 调整到 25°C，同时保持原始聚合物能量密度的~80%，并在可达到的温度下实现自修复（~ 70°C）。通过使用这种可自修复的高能 SMP，我们实现了宏观薄膜损伤（例如厘米大小的刀刺伤）的快速愈合，而在没有高能形状记忆辅助自修复 (SMASH) 的情况下，聚合物中无法修复这种损伤行为。自修复SMP用于制造具有高循环性和灵敏度的自修复力传感器，标志着在为智能、耐用可穿戴设备创建可调谐和自修复SMP方面取得了重大进步。