This chapter mainly focuses on the efficient use of ionic liquids for functionalization and materialization of natural polysaccharides. As ionic liquids are known to exhibit good affinity for polysaccharides, they have been employed in a variety of polysaccharide research studies. Although natural polysaccharides such as cellulose and chitin often show poor solubility in water and common organic solvents, ionic liquids have been found to act as good solvents for them. Accordingly, ionic liquids form ion gels with various polysaccharides via appropriate procedures from solutions. These ion gels can be further converted into value-added materials such as hydrogels, nanofibers, and films. Furthermore, a cellulose/chitin binary ion gel has been used as an electrolyte for an electric double layer capacitor. Because polymerizable ionic liquids also show good affinity for polysaccharides, in situ polymerization in the presence of polysaccharides has efficiently produced composite materials with polymeric ionic liquids. The resulting polysaccharide materials combined with ionic liquids show unique and high performance properties, e.g., shape memory, specific fluorescence emission, and high electrical conductivity.