Temperature‐Induced Morphological Transitions for On‐Demand Detachment in Worm‐Based Polymer Hydrogels

Temperature‐responsive materials are vital for applications relating to on‐demand detachable adhesives, as they enable rapid, damage‐free detachment. However, low‐temperature responsive systems often lack pronounced phase change, which can lead to undesirable mechanical interlocking with complicated substrate interfaces. Polymerisation‐induced self‐assembly (PISA) has been effectively employed to fabricate worm‐like hydrogels exhibiting temperature‐induced phase transitions; however, its application in on‐demand detachment remains underexplored. Building on this, we leverage precise morphological tuning across a broad temperature range (1 to 70 °C) to modulate the hydrogel phase. Our hydrogel exhibits a reversible transition from a robust adhesive state at room temperature to a non‐adhesive liquid phase upon both cooling and heating. This approach overcomes the limitations associated with low‐ and high‐temperature responsive detachment on complex surfaces, thereby broadening its utility.