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• PNS is a sustainable filler to develop cost-effective PLA biocomposites. • PNS enhanced PLA thermal stability, viscoelastic response, and crystallinity. • High filler loading did not cause significant decay in mechanical properties. • Ball milling of PNS further improved PLA thermal properties and melt fluidity. • Thermal annealing enhanced HDT, stiffness and strength of biocomposites. Biodegradable polymer composites reinforced with agri-food lignocellulosic biowaste represent cost-effective and sustainable materials potentially able to replace traditional composites for structural, household, and packaging applications. Herein, the preparation of polylactic acid (PLA)/pecan (Carya illinoinensis) nutshell (PNS) biocomposites at high filler loading (50 wt%) is reported, alongside the effect of two environmentally friendly physical treatments, namely ball-milling of the filler and thermal annealing on biocomposites. PNS enhanced the thermal stability, the viscoelastic response, and the crystallinity of the polymer. Furthermore, filler ball-milling also increased the melt fluidity of the biocomposites, potentially improving melt processing. Finally, the presence of PNS remarkably enhanced the effect of thermal annealing in the compounds. In particular, heat deflection temperature of the biocomposites dramatically increased, up to 60 °C with respect to the non-annealed samples. Overall, these results emphasize the potential of combining natural fillers and environmentally benign physical treatments to tailor the properties of PLA biocomposites, especially for those applications which require a stiff and lightweight material with low deformability. [ABSTRACT FROM AUTHOR]