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Plastics offer innumerable societal benefits but simultaneously contribute to persistent environmental pollution, dominated by polyethylene (PE) and isotactic polypropylene (iPP). Melt blending and reformulating postconsumer PE andiPP into useful materials presents a promising recycling approach. However, such repurposed plastics are generally mechanically inferior due to an inability to efficiently separate polyolefins in mixed waste streams; phase separation of PE andiPP results in brittleness as a consequence of poor interfacial strength. Recently, we demonstrated that a small amount (1 wt%) of a poly(ethylene)-block-poly(ethyl ethylene-ran-ethylene)-block-poly(ethylene) (EXE) triblock copolymer, synthesized by low-cost anionic polymerization of 1,3-butadiene followed by solution hydrogenation, restores tensile toughness to levels equivalent to virgin polyolefins. Unfortunately, low-temperature solvent insolubility of EXE, driven by crystallization of the E blocks containing 1.5 ethyl branches per 100 backbone repeat units (EB), presents a challenge for industrial hydrogenation. Comparable toughness (ca. > 400% strain at break) was achieved in the present work with 1.5 ≤ EB ≤ 6.5, accompanied by reduced EXE crystallinity and dissolution in cyclohexane down to room temperature at the highest EB content. This remarkable toughening behavior is attributed to a synergy between chain entanglements between the E end blocks and semicrystalline PE homopolymer and formation of E block “crystal nodules” that prevent chain pullout, along with topological constraints between the X loops and semicrystallineiPP. Our findings overcome barriers to commercial production of EXE with existing industrial facilities, providing a cost-effective strategy for recycling PE andiPP.