Herein, nonwoven alkali modified flax substrates were coated with incremental levels of chitosan, followed by immobilization of tannic acid, via a facile "dip-coating" strategy to yield a unique hierarchal "triplex" hybrid biomaterial, denoted as "THB". The characterization of the physicochemical properties of THB employed complementary spectroscopic (IR, Raman, and NMR) techniques, which support the role of hydrogen bonding and electrostatic interactions between the components: chitosan as the secondary biopolymer coating and the tertiary adsorbed polyphenols. XRD and SEM techniques provide further structural insight that confirms the unique semicrystalline nature and porous hierarchal structure of the biocomposite. The THBs present a polyphenol kinetic release profile that follows the Korsmeyer-Peppas model that concurs with Fickian diffusion for heterogeneous polymer systems. Furthermore, these systems demonstrate a tailored solvent uptake capacity (up to 4 g/g) in aqueous PBS media. Antipathogenic activity tests revealed 95% elimination of pathogens (, , and ) at a dose of 50 mg for the THB system. The trend in the structure-property relationships for the THB systems indicates synergistic effects of electrostatic multiform interactions between protonated chitosan and the polyphenol units. Herein, we report of a unique hierarchal biomaterial via a facile design strategy for diversiform roles as responsive adsorbents for environmental remediation to biomedical applications (e.g., controlled release, topical administration, or antimicrobial surface coatings).
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