Ionic liquids (ILs) are promising nonderivatizing solvents for the dissolution of cellulose and lignin in biomass pretreatment processes, which are, however, retarded by sluggish dynamics. Recent investigations showed that cosolvents such as dimethyl sulfoxide (DMSO) can accelerate the dissolution dramatically. On the other hand, water is used as a common antisolvent to regenerate cellulose from solutions. To understand the co-/antisolvent effects in dissolving cellulose by ILs, we performed molecular dynamics simulations of the interfaces between an I-beta cellulose crystal and different solvent systems, including ILs, DMSO, water, and mixed solvent systems. The density profiles and pair energy distributions (PEDs) show that the anions interact much more strongly with the cellulose surface than the cations, which is responsible for the dissolution of cellulose. It was found that the number of chloride ions; in contact with cellulose does not cause the co-/antisolvent effect In contrast, the cellulose chloride PEDs are sensitive to the addition of molecular solvents, such as DMSO and water. Detailed analyses Show that multiple hydrogen-bond (HB) patterns are formed between chloride and the hydroxyl groups of cellulose that are noticeably changed in the presence of DMSO or water. A combined analyses of both the PEDs and HB patterns can provide valuable information about the enhancement of cellulose dissolution. The simulation results in this work present useful knowledge for the design of solvent systems for dissolving cellulose or other types of biomass.