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Polyamides are one of the most important polymers. Long-chain aliphatic polyamides could bridge the gap between traditional polyamides and polyethylenes. Here we report an approach to preparing sustainable ultra-strong elastomers from biomass-derived long-chain polyamides by thiol-ene addition copolymerization with diamide diene monomers. The pendant polar hydroxyl and non-polar butyrate groups between amides allow controlled programming of supramolecular hydrogen bonding and facile tuning of crystallization of polymer chains. The presence of thioether groups on the main chain can further induce metal–ligand coordination (cuprous-thioether). Unidirectional step-cycle tensile deformation has been applied to these polyamides and significantly enhances tensile strength to over 210 MPa while maintaining elasticity. Uniaxial deformation leads to a rearrangement and alignment of crystalline microstructures, which is responsible for the mechanical enhancement. These chromophore-free polyamides are observed with strong luminescence ascribed to the effect of aggregation-induced emission (AIE), originating from the formation of amide clusters with restricted molecular motions.

Ultra-strong long-chain polyamide elastomers with programmable supramolecular interactions and oriented crystalline microstructures