The study of natural materials inspires sustainable innovations, with biomimetics excelling in surface modification. Polydopamine (PDA) offers a promising approach for modifying cellulose nanocrystals (CNC), enhancing their compatibility with hydrophobic polymers by improving interfacial adhesion. In this work, the modification of CNC with PDA (CNC@PDA) significantly enhanced the compatibility between the nanocargoes and the cellulose acetate (CA) matrix. The CNC@PDA complex formation was suggested through a combination of FTIR analysis, particle size distribution measurements and