Polysaccharide-based nanosystem is an umbrella term for many areas within research and technology dealing with polysaccharides that have at least one of their dimensions in the realm of a few hundreds of nanometers. Nanoparticles, nanocrystals, nanofibers, nanofilms, and nanonetworks can be fabricated from many different polysaccharide resources. Abundance in nature, cellulose, starch, chitosan, and pectin of different molecular structures are widely used to fabricate nanosystems for versatile industrial applications. This review presents the dissolution and modification of polysaccharides, which are influenced by their different molecular structures and applications. The dissolution ways include conventional organic solvents, ionic liquids, inorganic strong alkali and acids, enzymes, and hydrothermal treatment. Rheological properties of polysaccharide-based nano slurries are tailored for the purpose functions of the final products, e.g., imparting electrostatic functions of nanofibers to reduce viscosity by using lithium chloride and octenyl succinic acid to increase the hydrophobicity. Nowadays, synergistic effects of polysaccharide blends are increasingly highlighted. In particular, the reinforcing effect of nanoparticles, nanocrystals, nanowhiskers, and nanofibers to hydrogels, aerogels, and scaffolds, and the double network hydrogels of a rigid skeleton and a ductile substance have been developed for many emerging issues.