Abstract: With the current scenario of green chemistry looming large, biocomposites comprising cellulose and polyvinyl alcohol were synthesized using a non-toxic crosslinker, tetraethyl orthosilicate. Surface modification of the aforementioned composites was performed by non-thermal argon plasma. The plasma treatment rendered the composites hydrophilic; evident from the contact angle, surface free energy, swelling and FTIR studies. X-ray diffractrograms revealed plasma treatment did not hamper the organization of the polymer chains in the composites. With increasing hydrophilicity, the polymeric matrix acquired a more porous morphology. More so, enhanced surface roughness was also witnessed post-plasma treatment. The composites exhibited good antimicrobial activity against gram-positive bacterium S. pyogenes. Ibuprofen release studies from the composites validate their drug delivery potential. Hemolytic experiments confirm that plasma treatment does not evoke any detrimental effects on the structure of blood cells. Cytotoxicity assessment on MCF-7 cells demonstrated the biocompatibility and high cell viability of the composites. The composites were found to be remarkably biodegradable. Surface modified cellulose/polyvinyl alcohol composites by non-thermal Ar plasma are indeed potent for myriad applications towards biological relevance.Graphical abstract: