Due to environmental concerns increasing attention is focused on the application and preparation of bio-based polymers and their blends. In this study, cellulosethe most spread biopolymer on Earth, has been used in the preparation of novel cotton/polypropylene-Au and cotton/polyethylene-Au nanocomposites via green mechanochemical approach. First, mechanoradicals were generated by ball milling of cotton and thermoplastics in cryo conditions, then, these radicals were used in the reduction of gold ions to gold nanoparticles (Au NPs). Nanocomposites were characterized by Scanning Electron Microscopy (SEM), X-Ray Diffraction (XRD), and X-Ray Photoelectron Spectroscopy (XPS). The application of mechanochemistry in obtaining cotton/thermoplastic blends allowed homogenous and fine blending of the samples and in addition, excluded the usage of toxic solvents. Since gold nanoparticles exhibit a wide range of applications e.g. in catalysis, cotton/thermoplastic-Au nanocomposites were used to catalyse the reduction reaction of 4-nitrophenol to 4-aminophenol followed by UV-Vis spectroscopy. Finally, the hydrophobicity of the nanocomposites was alternated by tuning the blend composition. In the prepared nanocomposites, cotton and thermoplastics act as very good supporting matrices for gold nanoparticles and give a satisfactory access to NPs.