Although polymers based on polylactic acid (PLA) are considered by researchers as prime candidates for replacing traditional plastics, they are confronted with challenges including high production costs, limited thermal stability, and inferior impact resistance. In this study, novel composites with exceptional impact resistance, robust thermal stability, and satisfactory crystalline properties were fabricated by using PLA and polypropylene (PP) as raw materials, PP-g-MAH was employed as a compatibilizer to enhance the compatibility between the individual components. by adjusting the quantity of discarded cotton stalk fibers (CSF). The optimal mass ratio of CSF was determined to be 20%, resulting in a composite that exhibited a moderate increase of 56.31% in impact strength and a remarkable improvement of 23.05% in Vicat softening temperature. While the crystallinity was enhanced and the crystallization temperature (Tc) value decreased, the storage modulus also increased. Furthermore, the observed increase in storage modulus within the temperature range of 80 °C–100 °C was attributed to the influence of polymer cold crystallization. The hydrophobicity of the composite was enhanced. Significantly, this strategy can be extended to the application of other plant fibers, improving the crystalline properties of semi-crystalline polymers such as PLA and exemplifying the true ‘valorization of waste' through the secondary utilization of discarded CSF.