The development of supramolecular materials has opened up unprecedented opportunities for smart, responsive systems. Yet, their practical application in extreme environments-deep space, deep sea, polar regions, high-temperature and high-pressure reservoirs-is fundamentally challenged by the inherent trade-off between structural stability and dynamic adaptability. This review addresses this core issue by presenting a comprehensive framework for understanding and overcoming the stability-dynamism mismatch under harsh condition. We systematically analyze the molecular mechanisms by which severe factors disrupt non-covalent networks. Based on these insights, we outline four universal molecular design strategies that re-establish the balance, and summarize engineering applications across aerospace, marine, energy, and polar exploration. Beyond offering a comprehensive roadmap for rational material design, this review highlights persistent challenges-including multi-field coupling failure mechanisms, industrialization barriers, and the limitations of current systems-and outlines future directions. By bridging fundamental chemistry with extreme environment engineering, this work aims to guide the next generation of supramolecular materials that can reliably serve in the most demanding operational scenarios.
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