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In this work, the effect of long-chain branching (LCB) on the tensile properties of sulfur-cured, unfilled, polypentenamer rubber (PPR) was investigated. Branched PPR, prepared by ring-opening metathesis copolymerization of cyclopentene (CP) and dicyclopentadiene (DCPD), showed improved mechanical strength, demonstrating more than 3 times higher tensile stress at 500% strain compared to its linear counterpart (a homopolymer of CP). In situ wide-angle X-ray scattering showed that branching units caused significant changes in the strain-induced crystallization (SIC). At low temperatures, linear PPR underwent rapid SIC after a critical stretch was reached, while branched PPR crystallized more slowly. However, SIC is not the cause of the enhanced mechanical strength. Elevated temperature experiments confirmed that even in the absence of SIC, LCB PPR exhibits a stiffer stress–strain response. We propose …