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In the present study, polymer sponges based on poly(vinyl alcohol) (PVA) were prepared for the topical wound administration of chloramphenicol (CHL), an antibiotic widely used to treat bacterial infections. Nanocellulose fibrils (CNF) were homogenously dispersed in PVA sponges in three different ratios (2.5, 5, and 10 wt %) to improve the mechanical properties of neat PVA sponges. Infrared spectroscopy showed hydrogen bond formation between CNF and PVA, while scanning electron microscopy photos verified the successful dispersion of CNF to PVA sponges. The addition of CNF successfully enhanced the mechanical properties of PVA sponges, exhibiting higher compressive strength as the content of CNF increased. The PVA sponge containing 10 wt % CNF, due to its higher compression strength, was further studied as a matrix for CHL delivery in 10, 20, and 30 wt % concentration of the drug. X-ray diffraction showed that CHL was encapsulated in an amorphous state in the 10 and 20 wt % samples, while some crystallinity was observed in the 30 wt % ratio. In vitro dissolution studies showed enhanced CHL solubility after its incorporation in PVA/10 wt % CNF sponges. Release profiles showed a controlled release lasting three days for the sample containing 10 wt % CHL and 1.5 days for the other two samples. According to modelling, the release is driven by a pseudo-Fickian diffusion.