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Key relationships between molecular structure and final properties are reported for standard flow and high flow grades of commercially-available polyetheretherketone (PEEK) resins that differ primarily in molecular weight and molecular weight distribution. Despite similar chemistry and composition, the molecular size-dependent structural differences associated with the PEEK resins in this study are shown to influence the crystallization rate, final crystallinity, and melt rheology during processing, which subsequently affects mechanical properties, including strength, ductility, and impact resistance. These structure-property relationships provide fundamental understanding to aid in the design and manufacturing of industrial and medical devices that leverage both the advantages common to all PEEK resins, including chemical and thermal resistance, mechanical strength, and biocompatibility, as well as more subtle differences in crystallization kinetics, melt rheology, ductility, and impact resistance. POLYM. ENG. SCI., 2016. © 2016 Society of Plastics Engineers