There is a huge requirement of elastomers for use in tires, seals, and shock absorbers every year worldwide. In view of a sustainable society, the next generation of elastomers is expected to combine outstanding healing, recycling, and damage‐tolerant capacities with high strength, elasticity, and toughness. However, it remains challenging to fabricate such elastomers because the mechanisms for the properties mentioned above are mutually exclusive. Herein, the fabrication of healable, recyclable, and mechanically tough polyurethane (PU) elastomers with outstanding damage tolerance by coordination of multiblock polymers of poly(dimethylsiloxane) (PDMS)/polycaprolactone (PCL) containing hydrogen and coordination bonding motifs with Zn2+ ions is reported. The organization of bipyridine groups coordinated with Zn2+ ions, carbamate groups cross‐linked with hydrogen bonds, and crystallized PCL segments generates phase‐separated dynamic hierarchical domains. Serving as rigid nanofillers capable of deformation and disintegration under an external force, the dynamic hierarchical domains can strengthen the elastomers and significantly enhance their toughness and fracture energy. As a result, the elastomers exhibit a tensile strength of ≈52.4 MPa, a toughness of ≈363.8 MJ m−3, and an exceptional fracture energy of ≈192.9 kJ m−2. Furthermore, the elastomers can be conveniently healed and recycled to regain their original mechanical properties and integrity under heating.

Summary: A rather simple but yet effective way to achieve a superhydrophobic film by extending a Teflon film is proposed. The water‐contact angle can be increased from 118 to 165° by extending to ca. 190%. The fibrous crystals and the increasing distance between the fibrous crystals are believed responsible for the high water‐contact angle. It indicates that the density of the aligned microstructures is very important for the superhydrophobicity.Water‐contact angle and the corresponding shapes of water droplets as a function of extension ratio of Teflon tape.imageWater‐contact angle and the corresponding shapes of water droplets as a function of extension ratio of Teflon tape.

Polymeric materials used in spacecraft require to be protected with an atomic oxygen (AO)-resistant layer because AO can degrade these polymers when spacecraft serves in low earth orbit (LEO) environment. However, mechanical damage on AO-resistant coatings can expose the underlying polymers to AO erosion, shortening their service life. In this study, the fabrication of durable AO-resistant coatings that are capable of autonomously healing mechanical damage under LEO environment is presented. The self-healing AO-resistant coatings are comprised of 2-ureido-4[1H]-pyrimidinone (UPy)-functionalized polyhedral oligomeric silsesquioxane (POSS) (denoted as UPy-POSS) that forms hydrogen-bonded three-dimensional supramolecular polymers. The UPy-POSS supramolecular polymers can be conveniently deposited on polyimides by a hot pressing process. The UPy-POSS polymeric coatings are mechanically robust, thermally stable, and transparent and have a strong adhesion toward polyimides to endure repeated bending/unbending treatments and thermal cycling. The UPy-POSS polymeric coatings exhibit excellent AO attack resistance because of the formation of epidermal SiO layer after AO exposure. Due to the reversibility of the quadruple hydrogen bonds between UPy motifs, the UPy-POSS polymeric coatings can rapidly heal mechanical damage such as cracks at 80 °C or under LEO environment to restore their original AO-resistant function.