Highly sustainable composites were produced by melt compounding polylactide (PLA) with almond shell flour (ASF), a processed byproduct of the food industry, at a weight content of 30 wt.-%. However, due to the lack of miscibility between PLA and ASF, both being raw materials obtained from crops, resultant green composite presented poor ductility and low thermal stability. To overcome this limitation, maleinized linseed oil (MLO), a multi-functionalized plant-derived additive, was originally incorporated as a reactive compatibilizer during the extrusion process. Both chemical and physical characterizations showed that 1-5 parts per hundred resin (phr) of MLO successfully serve to function as a novel compatibilizer on the PLA/ASF composites, leading to highly sustainable materials with balanced mechanical, thermal, and thermomechanical properties. Achieved compatibilization was particularly related to a dual effect of plasticization in combination with grafting. The latter effect was ascribed to the formation of new carboxylic ester bonds through the reaction of the multiple maleic anhydride groups present in MLO with the hydroxyl terminal groups of both PLA chains and lignocellulose on the ASF surface. The fully bio-based and 2 biodegradable composites described herein give an efficient sustainable solution to upgrade agrofood wastes as well as contributing to reducing the cost of PLA-based materials.