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Thermoresponsive polymer brushes are grafted on micro/nanostructured polymer substrates as new intelligent interfaces that synergistically enhance wettability changes in response to external temperature stimuli. Thermoplastic poly(styrene-co-4-vinylbenzyl chloride) [P(St-co-VBC)] is synthesized using radical polymerization and spin-coated on a glass substrate. Micro/nanopillar and hole patterns are imprinted on the P(St-co-VBC) layer using thermal nanoimprint lithography. Poly(N-isopropylacrylamide) (PIPAAm) brushes are grafted on the micro/nanostructured P(St-co-VBC) layer through surface-initiated atom-transfer radical polymerization using 4-vinylbenzyl chloride as the initiator. The imprinted micro/nanostructures and grafted PIPAAm brush chain lengths affect the surface wettability. Combinations of nanopillars or nanoholes (diameter 500 nm) and longer PIPAAm brushes enhance hydrophobic/hydrophilic changes in response to temperature changes, compared with the flat substrate. The thermoresponsive hydrophobic/hydrophilic transition is synergistically enhanced by the nanostructured surface changing from Cassie-Baxter to Wenzel states. This PIPAAm-brush-modified micro/nanostructured P(St-co-VBC) is a new intelligent interface that effectively changes wettability in response to external temperature changes. [ABSTRACT FROM AUTHOR]

Front Cover: Thermoresponsive interfaces showing significant wettability changes are fabricated by nano‐imprinting a poly(styrene‐co‐4‐vinylbenzyl chloride) layer and subsequent surface‐initiated ATRP of N‐isopropylacrylamide. Combinations of nanopillars or nanoholes and longer poly(N‐isopropylacrylamide) brushes enhance hydrophobic/hydrophilic changes in response to temperature changes, compared with a flat substrate. The thermoresponsive hydrophobic/hydrophilic transition is enhanced by the nanostructured surface changing from Cassie‐Baxter to Wenzel states. Further details can be found in the article by K. Nagase,* T. Onuma, M. Yamato, N. Takeda,* and T. Okano* on page 1965. [ABSTRACT FROM AUTHOR]