The desire for lightweight, carbon-negative materials has been increasing in recent years, particularly as the transportation sector reduces its global carbon footprint. Natural fibers, such as flax fiber and their composites, offer a compelling combination of properties including low density, high specific strength, and carbon negativity. However, because of the low modulus and high variability in performance, natural fibers can’t compete with glass fibers as structural reinforcements in polymer composites. In this study, flax technical fibers were treated in supercritical CO2 (scCO2), and the effects of this treatment on the morphology and properties of flax fibers are reported. Treatment in scCO2 successfully resulted in higher fiber modulus and strength by 33% and 40%, respectively. Fiber porosity was reduced by 50% and morphological changes to the fibers were observed. Specifically, fiber lumen collapsed during treatment and micro/mesoporosity was reduced by 27%. Treated flax fibers were used to create 30 vol% unidirectional flax-epoxy composites. ScCO2 treatment raised composite modulus and strength by 33% and 25%, respectively. Because of the dependence between technical fiber size and mechanical properties, the relationship between fiber modulus and fiber size were created and applied to the rule-of-mixtures. This relationship were found to be viable representations of the fiber performance within each composite. Overall, the treatment developed in this study has the potential to significantly improve natural fiber properties, enabling their consideration for use in lightweight, semi-structural composites.