<p dir="ltr">Recent advances in materials have opened new opportunities for wearable healthcare, human–machine interactions, and robotics. Their real-world adoption remains limited by insufficient durability across mechanical, electrical, environmental, and thermal aspects, leading to issues such as fracture, freezing, dehydration, and thermal instability. To address these challenges, I engineered materials at multiple scales (e.g., micro-, nano-, and molecular-levels), by establishing novel “process–structure–property” relationships, to explore their extreme properties in terms of mechanical, environmental, electrical and thermal perspectives. These materials are evaluated through computational simulations and integrated into wearables for reliable healthcare. I will introduce the design principles of the durable materials, including tough hydrogels, environmentally resilient hydrogels, self-healing hydrogels, and stretchable spongy foams for reliable health monitoring.</p>