The aim of the study was to find new structured biopolymer blends bearing adjustable properties able to produce innovative materials. Apart from cellulose and three solvents (NaOH, N-methylmorpholine-N-oxide [NMMO] and 1-ethyl-3-methylimidazolium acetate [EMIMac]), 15 different polysaccharides were chosen to study the interactions ofpolysaccharides or their mixtures in solutions, as well as the solid state after forming. Dissolution screenings yielded promising polysaccharides, which were used for the preparation of cellulose/ polysaccharide solutions and subsequently for the shaping of blends with cellulose. The solubility and miscibility were evaluated by microscopy, DSC, particle analysis and rheology. Polysaccharides with a structure similar to that of cellulose, e.g., xylan, carrageenan or cellulose carbamate were not miscible, showing globular morphologies, whereas high-molar and side chains containing polysaccharides such as xanthan or tragacanth gum form co-continuous morphologies. The forming of blend fibres was nevertheless possible for all three solvents. The textile-physical properties of the blend fibres were slightly decreased compared to those of the unmodified fibre, in which fibres from NMMO and EMIMac had the highest performance. The presence of blended polysaccharides in the fibres produced was verified by residue sugar analysis, in which the highest amounts occurred for EMIMac fibres.