Recently, the demand for the use of natural polymers in the cosmetic, biomedical, and sanitary sectors has been increasing. In order to meet specific functional properties of the products, usually, the incorporation of the active component is required. One of the main problems is enabling compatibility between hydrophobic and hydrophilic surfaces. Therefore, surface modification is necessary. Poly(lactide) (PLA) is a natural polymer that has attracted a lot ofattention in recent years. It is bio-based, can be produced from carbohydrate sources like corn, and it is biodegradable. The main goal of this work was the functionalization of PLA, inserting antiseptic and anti-inflammatory nanostructured systems based on chitin nanofibrils–nanolignin complexes ready to be used in the biomedical, cosmetics, and sanitary sectors. The specific challenge of this investigation was to increase the interaction between the hydrophobic PLA matrix with hydrophilic chitin–lignin nanoparticle complexes. First, chemical modification via the “grafting from” method using lactide oligomers was performed. Then, active coatings with modified and unmodified chitin–lignin nanoparticle complexes were prepared and applied on extruded PLA-based sheets. The chemical, thermal, and mechanical characterization of prepared samples was carried out and the obtained results were discussed.