Catastrophically mechanical failure of soft self-healing materials is unavoidable due to their inherently poor resistance to crack propagation. Here, with a model system, i.e., soft self-healing polyurea, we present a biomimetic strategy of surpassing trade-off between soft self-healing and high fracture toughness, enabling the conversion of soft and weak into soft yet tough self-healing material. Such an achievement is inspired by vascular smooth muscles, where core-shell structured Galinstan micro-droplets are introduced through molecularly interfacial metal-coordinated assembly, resulting in an increased crack-resistant strain and fracture toughness of 12.2 and 34.9 times without sacrificing softness. The obtained fracture toughness is up to 111.16 ± 8.76 kJ/m², even higher than that of Al and Zn alloys. Moreover, the resultant composite delivers fast self-healing kinetics (1 min) upon local near-infrared irradiation, and possesses ultra-high dielectric constants (~14.57), thus being able to be fabricated into sensitive and self-healing capacitive strain-sensors tolerant towards cracks potentially evolved in service.

软质自愈材料的灾难性机械故障是不可避免的，因为它们本身对裂纹扩展的抵抗力很差。在这里，我们利用一种模型系统，即柔软的自愈聚脲，提出了一种超越软自愈和高断裂韧性之间权衡的仿生策略，能够将软而弱的材料转化为柔软而坚韧的自愈材料. 这一成就受到血管平滑肌的启发，通过分子界面金属配位组装引入核壳结构的 Galinstan 微滴，从而在不牺牲柔软性的情况下将抗裂应变和断裂韧性提高了 12.2 倍和 34.9 倍。获得的断裂韧性高达111.16 ± 8.76 kJ/m ²，甚至高于铝和锌合金。此外，所得复合材料在局部近红外辐射下具有快速自愈动力学（1 分钟），并具有超高介电常数（~14.57），因此能够制成灵敏且自愈的电容式应变传感器容忍在服务中可能出现的裂缝。