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The effects of surface treatment of flax fibers featuring vinyltrimethoxy silane (VTMO) and maleic anhydride-polypropylene (MAPP) on the mechanical properties of flax/PP composites were investigated. α-polypropylene (α-PP) and β-polypropylene (β-PP) were used as matrices for measuring the mechanical properties of the flax fiber/polypropylene (flax/PP) composites. Flax/PP composites composed of double-covered uncommingled yarn (DCUY) were prepared using a film-stacking technique. The influence of surface treatment on the tensile, flexural, impact, and water uptake properties of Flax/PP composites were investigated. MAPP treatment was suitable for flax/PP composites in terms of superior tensile and impact properties. VTMO treatment showed superior flexural properties and less influence on the impact properties after moisture absorption.