All-cellulose composites (ACCs) are a promising new class of bio-composites which emerged to overcome especially the critical problem of adhesion in composites and to substitute the conventional petroleum-based polymers. Different processing routes have been used to develop these bio-materials, based on partial or complete solubilisation using different solvent systems. However, the potential industrial applications remain limited due to the using of hazardous and expensive solvents and to difficulties in controlling the consolidation mechanism in cellulose during regeneration. The aim of the present work is to develop a high-performance composite using biomimetic approaches that will exploit the fundamental interactions between two bio-polymers, cellulose and xyloglucan, and these interactions are typically present within the cell walls of plants, according to the “tethered network” model. In this study, the attractive solubilisation potential of ionic liquids is used to co-dissolve and to prepare cellulose-xyloglucan blends. Films of regenerated cellulose, xyloglucan and various cellulose/xylogucan blends were prepared using [EMIM] Acetate or Choline acetate-DMSO as a co-solvent. The raw materials and regenerated composite films were characterized by chemical analysis, X-ray diffraction, FTIR, solid NMR, morphology, hygro-mechanical analysis and tensile testing. In terms of mechanical properties, a synergy could be observed in the regenerated blends with an increase of both modulus and elongation at break compared to the regenerated pure biopolymers. Strategies for upscaling the production to thick composite laminates will also be discussed. Keywords: Cellulose, xyloglucan, ionic liquids, polymers blends, biomimetic approaches, hydro-mechanical properties.