To accurately predict the crystal morphologies of dihydroxylammonium 5, 5′-bistetrazole-1, 1′-diolate (HATO, also known as TKX-50) under different growth conditions, the PCFF force field parameters were systematically validated and modified. The attachment energies of HATO crystal surface were calculated by the molecular simulation method. The crystal morphologies of HATO in vacuum, in seven solvents (water, dimethyl sulfoxide, methanol, ethanol, ethyl acetate, tetrahydrofuran and trichloromethane), and in three additives (sodium laurylsulfonate, sodium dodecyl benzene sulfonate and dextrin) were obtained. Results show that the crystal morphology of HATO in a vacuum is long flaky, consisting of five cryatal faces, (0 2 0), (1 1 -1), (0 1 1), (1 1 0) and (1 0 0), among them, cryatal face (0 2 0) is the most important, occupying the 53.97% of total surface area. In the polar solvents, including dimethyl sulfoxide, methanol, and ethanol, the morphological importance of (0 2 0) cryatal face decreases, the crystal morphology of HATO is improved. In the three additives, the crystal morphology of HATO is still long flaky. The predicted structure of crystal morphology of HATO is in good agreement with the experiments, it can provide theoretical guidance for the crystal morphology control of HATO.