Crystalline polysaccharides, which are abundant in nature, can be transformed into highly functional materials. However, the molecular basis for the formation of higher-order structures remains incompletely understood. Computer simulation is an advanced tool for modeling macromolecular structures, with atomistic simulations providing valuable information on crystalline polysaccharides. This focus review covers theoretical and computational studies, including atomistic simulations, performed by our research group on the crystallographic properties and novel nanostructures of cellulose, crystal structure of amylose analog polysaccharides, and dissolution mechanism of cellulose and chitin crystalline fibers.
