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Paper-based food packaging materials are widely used, renewable, and biodegradable. Because of its porous structure, paper has poor or no barrier performance against grease, water vapor, water, and volatile organic compounds. Moreover, recycled paperboard can be a source of organic residuals that are able to migrate into packed food. Two different types of paperboard produced from primary and secondary cellulosic fibers were coated using renewable materials, such as alginate and chitosan, and comprehensive barrier measurements showed multifunctional barrier properties of these two biomaterials. Both paper substrates were successfully coated using a draw-down coater, and the measured air permeability of the coated samples was 0 mL·min⁻¹. Grease resistance was improved, while it was possible to reduce water vapor transmission, the migration of mineral oil saturated hydrocarbons and mineral oil aromatic hydrocarbons (MOSH/MOAH), and the permeation of volatile compounds for both paper substrates when compared with uncoated substrates. Wettability and water absorptiveness of chitosan- and alginate-coated papers were found to be substrate-dependent properties, and could be significantly affected by bio-based coatings. In summary, industrially produced paperboard was upgraded by coating it with the naturally biodegradable biopolymers, alginate and chitosan, thus achieving extraordinary barrier performance for various applications within the packaging industry. Full article