| Summary: | This study describes the fabrication of bioinspired mechano‐regulated interfaces (MRI) for the separation and collection of oil spills from water. The MRI consists of 3D‐interconnected, microporous structures of sponges made of ultrasoft elastomers (Ecoflex). To validate the MRI strategy, ecoflex sponges are first fabricated with a low‐cost sugar‐leaching method. This study then systematically investigates the absorption capacity (up to 1280% for chloroform) of the sponges to different oils and organic solvents. More importantly, the oil flux through the as‐made sponges is controlled by mechanical deformation, which increases up to ≈33‐fold by tensile strain applied to the sponge from 0 to 400%. On the basis of MRI, this study further demonstrates the application of ecoflex sponges in oil skimmers for selective collecting oil from water with high efficiency and durable recyclability. The as‐developed MRI strategy has opened a new path to allow rational design and dynamical control toward developing high performance devices for oil permeation and selective collection of oil spills from water.
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