A Versatile Microporous Design toward Toughened yet Softened Self‐Healing Materials

Realizing the full potential of self-healing materials in stretchable electronics necessitates not only low modulus to enable high adaptivity, but also high toughness to resist crack propagation. However, existing toughening strategies for soft self-healing materials have only modestly improves mechanical dissipation near the crack tip (Г_D), and invariably compromise the material's inherent softness and autonomous healing capabilities. Here, a synthetic microporous architecture is demonstrated that unprecedently toughens and softens self-healing materials without impacting their intrinsic self-healing kinetics. This microporous structure spreads energy dissipation across the entire material through a bran-new dissipative mode of adaptable crack movement (Г_A), which substantially increases the fracture toughness by 31.6 times, from 3.19 to 100.86 kJ m^-2, and the fractocohesive length by 20.7 times, from 0.59 mm to 12.24 mm. This combination of unprecedented fracture toughness (100.86 kJ m^-2) and centimeter-scale fractocohesive length (1.23 cm) surpasses all previous records for synthetic soft self-healing materials and even exceeds those of light alloys. Coupled with significantly enhanced softness (0.43 MPa) and nearly perfect autonomous self-healing efficiency (≈100%), this robust material is ideal for constructing durable kirigami electronics for wearable devices.