Blends based on polylactic acid (PLA), chitosan, and grape seed extract (GE) were prepared by extrusion and injection molding. The effect of chitosan (5% and 15% on PLA basis) and natural extract (1% on PLA basis) incorporated into the PLA host matrix was explored regarding the thermal and mechanical properties. GE showed antioxidant activity, as determined by the DPPH assay method. Chitosan and GE affect the degree of crystallinity up to 30% as the polysaccharide acts as a nucleating agent, while the extract reduces the mobility of PLA chains. The decomposition temperature was mainly affected by adding chitosan, with a reduction of up to 25 °C. The color of the blends was specially modified after the incorporation of both components, obtaining high values of b* and L* after the addition of chitosan, while GE switched to high values of a*. The elongation at break (EB) exhibited that the polysaccharide is mainly responsible for its reduction of around 50%. Slight differences were accessed in tensile strength and Young’s modulus, which were not statistically significant. Blends showed increased irregularities in their surface appearance, as observed by SEM analysis, corresponding to the partial miscibility of both polymers.

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