In the present investigation, a novel, green, and economical dual-functionalized pullulan/kaolin hydrogel nanocomposite (f-PKHN) was fabricated and subsequently applied for the liquid-phase decontamination of paracetamol (PCT), a pharmaceutical pollutant. Pullulan and kaolin were functionalized with L-asparagine and gallic acid, respectively. The physicochemical facets of the functionalized pullulan/kaolin hydrogel nanocomposite and its interactive behavior with PCT were elucidated by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), scanning electron microscopy-energy dispersive X-ray spectroscopy (SEM-EDX), and elemental mapping. The process parameters along with the isotherm, kinetics, and thermodynamics were methodically appraised via a batch technique to unveil the adsorption performance of the as-fabricated hydrogel nanocomposite. The adsorption isotherm and kinetics of PCT uptake by f-PKHN conform well to Freundlich and pseudosecond-order models, respectively. Relying on hydrogen bonding, n−π, and van der Waals interactions, the maximum adsorption capacity was 332.54 mg g −1 , higher than for most of the previous adsorbents reported in the literature for PCT removal. Thermodynamic calculations corroborated endothermic, spontaneous, and feasible adsorption phenomena. The maintenance of a high uptake percentage (69.11%) in the fifth consecutive adsorption−desorption cycle implied the significant reusable potential of f-PKHN. Swelling studies exhibited 90% swelling within 200 min, indicating the successful fabrication of a cross-linked hydrogel network. The real water (distilled water, tap water, and river water) samples spiked with PCT specified a significant uptake of PCT (>85%), and the minor influence of ionic strength on the adsorptive potential of f-PKHN validated its potentiality for the decontamination of real effluents. In conclusion, f-PKHN with substantial adsorption capacity, green characteristics, and excellent reusability can be reckoned with as a promising adsorbent for the de-escalation of PCT from aquatic sources as well as at the industrial level.
