Considering the environmental and more stringent legislative pressures (at least in the EU), there is a pressing need for innovative, sustainable and recyclable materials. Therefore, the industry needs to move to greener materials that meet the physical performance of the conventional engineering materials. One of the most suitable and most abundant renewable materials able to fulfil this requirement is cellulose. Cellulose is a linear polysaccharide chain synthesized by plants or bacteria. We are aiming to produce composites, which combine cellulose from different origins in order to obtain an all-cellulose hierarchical composite structure. The different cellulose types used are commercially available microcrystalline cellulose powder, technical lignocellulosic fibres and bacterial cellulose. The bacterial cellulose was produced by bacterial synthesis using an Acetobacter Xylinum strain (BRP 2001) in highly ordered fashion, whereas, the plant cellulose is a semicrystalline polymer which also contains some other compounds like pectin, waxes and hemicellulose. The crystalline cellulose powder was dissolved in a non-derivative co-solvent (dimethylacetamide/LiCl) and subsequently regenerated to form the cellulose matrix. Natural (lignocellulosic) fibres were used as reinforcement. The natural fibre surfaces were modified by depositing nano-sized bacterial cellulose onto the fibres during the bacterial synthesis in presence of the fibres. This modification does not lead to any apparent mechanical degradation of the fibres. The attaching bacterial cellulose to the fibres enhances the effective fibre surface area of the fibres which is anticipated to lead to greater interaction with the regenerated cellulose matrix. The composite performance can be tailored by tuning the degree of crystallinity of the regenerated cellulose matrix, which is a function of the processing time during dissolution. It is anticipated that this type of composite materials can be produced using recycled paper as the cellulose source to produce the matrix of the composite. All-cellulose hierarchical composites might be able to substitute traditional based glass fibres reinforced polymers in a near future.