In this paper, a molecular model for adsorption of NTO surface-solvent was constructed, and the effects of different solvents on the morphology of NTO crystal were simulated by molecular dynamics. The selected solvents included ethanol, water, acetone, N-methylpyrrolidone (NMP), ethyl acetate and N,N-dimethylformamide. Pure solvents and two co-solvents including NMP/water and ethanol/water were studied to provide theoretical guidance for the selection of solvent systems for NTO recrystallization. In pure solvents, the results show that the crystal morphology of NTO can be effected by all solvent and in NMP solvent is the best. In co-solvents, when the mass ratio of ethanol to water is 9:1, the best morphology of NTO crystals is found . In ethanol/water system, the morphology of NTO crystals changes from near-cube to cuboid with the decrease of ethanol mass fraction, and the aspect ratios of NTO crystals increase. In NMP/water system, the decrease of the mass fraction of NMP makes the crystal morphology deteriorate. This is manifested as the crystal develops towards a narrow needle shape, and the value of the aspect ratio increases.