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The aim of this work is to study the influence of low-pressure plasma treatment on cellulose fibres to improve the adhesion between a polymeric matrix and natural fibres used as reinforcement. To evaluate fibre wettability, contact angle measurements were carried out on flax fibres after treatment with plasma under several conditions. Similarly, contact angle measurements were performed without plasma treatment. A comparison between all the samples led to the definition of the optimal plasma treatment conditions. Once the latter were determined, composite materials were prepared with treated and untreated flax fibres and a low-density polyethylene matrix. Composites, with different fibre contents (5 and 40%) and different fibre lengths (1 and 10 mm), were manufactured using a mixer and a hot plate press. The tensile strengths of the composites were assessed to determine optimal fibre content and length, and the plasma treatment effect was also quantified. It was found that the higher the fibre content, the higher the tensile strength, and the higher the Young's modulus; however, fibre length did not affect tensile strength. Regarding plasma treatment, composites with treated fibres exhibited a considerably improved tensile strength and Young's modulus. Plasma treatment effects were also studied by X-ray photoelectron spectroscopy and by differential scanning calorimetric. Finally, an analysis of the fibre surface and an interaction study between the matrix and the fibres was conducted with scanning electron microscopy.