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In this study, an effective strategy to significantly improve the mechanical properties of ductile polymers by simply adding a complimentary rigid polymer is introduced. This work uses a semi\u2010crystalline polymer aliphatic polyketone (POK) as the matrix material and a small quantity of polymethyl methacrylate (PMMA) as the rigid polymer, through establishing molecular chain entanglements at the interface to produce POK\/PMMA blends with exceptional mechanical property. The experimental study shows that PMMA as a small island phase is homogeneously dispersed in the POK matrix, while the interfacial adhesion between the POK matrix and PMMA island is enhanced by the high\u2010density molecular chain entanglement between PMMA and the POK matrix. The strong entanglements and high concentration of PMMA domains promote uniform crazes and overall shear yielding. As a result, the POK\/PMMA blend exhibits exceptional mechanical properties with notched impact strength, elongation at break, tensile strength, and Young's modulus, of 20\u00a0kJ\u00a0m<jats:sup>\u22122<\/jats:sup>, 326%, 60 and 2185\u00a0MPa, respectively. A universal approach is further suggested for enhancing the toughness and strength of ductile polymers using a complimentary rigid polymer.<\/jats:p>","DOI":"10.1002\/marc.202400886","type":"journal-article","created":{"date-parts":[[2025,1,15]],"date-time":"2025-01-15T12:40:17Z","timestamp":1736944817000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":7,"title":["Simultaneous Toughening and Strengthening of Ductile Polymer by Rigid Polymeric Fillers: The Role of Interfacial Entanglement"],"prefix":"10.1002","volume":"46","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-5045-0160","authenticated-orcid":false,"given":"Zichun","family":"Zhu","sequence":"first","affiliation":[{"name":"Department of Materials Science and Engineering National University of Singapore (NUS)  9 Engineering Drive 1 Singapore 117575 Singapore"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xunan","family":"Hou","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering National University of Singapore (NUS)  9 Engineering Drive 1 Singapore 117575 Singapore"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yongchao","family":"Liu","sequence":"additional","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Functional Soft Condensed Matter School of Materials and Energy Guangdong University of Technology  Guangzhou 510006 P. 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