The crystal morphologies of 3,4-bis(3-nitrofurazan-4-yl)furoxan (DNTF) are diamond-shaped in methanol as well as in acetic acid/water (7 : 3) solutions. There is a possibility that the two solutions have similar effects on the morphologies of DNTF. To explain this phenomenon, a spiral growth model in consideration of adhesion energy, temperature, solubility, and supersaturation was implemented to predict the crystal morphologies of the DNTF in the two solutions. The interface model based on the experimental situation was constructed as a periodic supercell. The molecular dynamics simulation was performed to obtain the attachment energy at the equilibrium structure. The results indicate that the (001), (111) and (111? ) faces become dominantly exposed faces, while the (011), (101) and (110) faces disappear or occupy a very small area in both solutions. The prediction results are in remarkable agreement with the experimental observations in cooling crystallization. The simulation method can provide theoretical support for the crystallization process of DNTF.