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Nanotechnology is making exceptional progress in the medical field. The development of new systems for the delivery of plant ingredients brings benefits such as good bioavailability, solubility, sustained release, and enhanced potential. To the best of our knowledge, there is no report on nanocomposites from Tetrapleura tetrapteradespite its wide range of ethnopharmacological uses including management of inflammatory diseases. This study aimed to prepare chitosan- and cellulose-based nanocomposites with anti-inflammatory potential. The biocomposites showed an encapsulation efficiency of 69.4%. Their formation was confirmed by a peak at 290 nm in UV–Vis. Infrared spectrophotometry proved the formation of a mixed polysaccharide and polyphenol system. No signs of toxicity and no deaths were found; therefore, the lethal dose 50 (LD50) is higher than 2000 mg/kg. The biocomposite has an anti-inflammatory activity in vitro with a maximum inhibition of 99.5% and an anti-inflammatory activity in vivo with a maximum inhibition of 98.7% for a dose of 200 mg/kg. The synthesized biocomposites from the aqueous extract of the fruits of Tetrapleura tetrapterashowed an anti-inflammatory property with satisfactory safety.