The aim of the present work is to develop a high-performance composite using biomimetic approaches that will exploit the interactions between two biopolymers, cellulose and xyloglucan, and these interactions play an important role but still not fully understood in the biomechanical properties of primary plant cell walls. In this study, the co-solubility of cellulose and xyloglucan in an ionic liquid (1-ethyl-3-methylimidazolium acetate (EMIMAC)) is used to prepare regenerated films by subsequent precipitation with a non-solvent. Films of pure cellulose, pure xyloglucan and various cellulose/xylogucan blends were obtained and characterized by Fourier transform-infrared spectroscopy (FTIR), X-ray diffraction (XRD) and hygro-mechanical analysis. The biopolymer blends show an increase of the storage modulus comparatively to the regenerated pure biopolymers.