The use of eco-friendly bioplastics has become a viable solution to reduce the accumulation of petrochemical products in the biosphere and to decrease microplastic contamination. In this study, we used low-quality cotton fibers that lack textile applications to prepare bioplastics. We dissolved cotton fibers in N,N-dimethylacetamide/lithium chloride (DMAc/LiCl) solvent system and converted cellulose solutions to strong, transparent, and flexible films through casting, gelation, regeneration, plasticization, and hot-pressing. Films were characterized using different analytical techniques to evaluate their physicochemical and mechanical properties. Compared to raw cotton cellulose, regenerated and hot-pressed cellulose films showed amorphous structures and excellent tensile characteristics. The physical and mechanical properties of cellulose films, such as deformation recovery, flexibility, homogeneity, elongation, and surface roughness, were significantly improved by means of plasticization and hot-pressing. Because glycerol plasticization increased the surface hydrophilicity of the films, plasma-induced surface grafting of oleic acid imparted hydrophobicity to cellulose films. This study presents a new avenue for using low-quality cotton fibers that are usually sold at a discounted price to produce value-added bioproducts for different applications. Graphic abstract