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posted on 2025.06.13 at 09:52:53 (c=0, p=3)
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Natural rubber, with annual production of 15 million tonnes, is the most used bio-elastomer. Improving its resistance to crack growth is highly desired, to prolong its service life for many applications and eventually improve its sustainability. Here we markedly amplify the resistance to crack growth in natural rubber by forming a tanglemer, a polymer network in which entanglements greatly outnumber crosslinks. Specifically, we cast natural rubber latex without high-intensity processing that cuts long polymers. The long polymers densely entangle by thermal motion and are then sparsely crosslinked. At a crack tip, long polymer strands between neighbouring crosslinks deconcentrate stress, extend strain-induced crystallization over a large region and enhance crystallinity. For example, when the ratio of crosslinks to repeat units reduces from 10β2 to 10β3, the network amplifies fatigue threshold from ~50βJβmβ2 to ~200βJβmβ2, and toughness from ~104βJβmβ2 to over 105βJβmβ2. Overall, this work provides a viable strategy to improve the practical applicability of natural rubber, contributing to the development of sustainable polymers. Natural rubber is a widely used biopolymer and further improving its resistance to crack growth will extend its service life. Here the authors show a strategy to amplify the resistance to crack growth in natural rubber by forming a tanglemer.