The theoretical crystal-morphology of zinc tricarbohydrazide perchlorate (ZnCP) was studied using the morphology simulation software. The growth trends and surface characteristics were calculated using the Bravais-Friedel-Donnay-Harker (BFDH), Growth Morphology, and Equilibrium Morphology methods; these provide theoretical guidance for the choice of crystal-control reagents. On the basis of the simulations, experiments were carried out to study the effects of five different crystal-control reagents, including carboxymethylcellulose (A), polyacrylamide (B), dextrin (C), Tween 40 (D), and Tween 60 (E), in the control of the crystal-morphology of ZnCP. Mixtures of two reagents and higher temperatures were used to further optimize the ZnCP crystals. The results show that ZnCP crystals are well dispersed, and have a large apparent density and regular crystal-morphology under the control of a mixture of reagents A and E in a mass ratio of 1:4 at 80°C. The crystal-morphology of an energetic material has a direct effect on its physical properties such as fluidity, apparent density, electrostatic accumulation, and pressure resistance, and even has an important impact on its chemical and explosive properties such as stability, detonation ability, and sensitivity [1,2]. Generally, a material with a smooth surface, uniform particles, and spherical crystals has many advantages over needle-or twig-like irregular crystals, such as good fluidity, high apparent density (more than 0.8 g/cm 3 ), low sensitivity, and stable performance [3,4]. A fine crystal-morphology plays an important role in the safety and stability of a material [5][6][7]. Methods for controlling crystal-morphology can therefore be used to regulate nucleation and crystal growth during the crystallization process to increase the production and use of security of energetic materials, and improve their energy output performances [8][9][10][11][12]. Zinc tricarbohydrazide perchlorate ([Zn(CHZ) 3 ](ClO 4 ) 2 , ZnCP) is a new green energetic coordination compound that excludes toxic heavy metals [13]. However, ZnCP crystals prepared using traditional synthetic techniques are too small, fragmented, and irregular, and have poor fluidity and a small apparent density (less than 0.7 g/cm 3 ), leading to weak explosive power. Crystal-morphology control using a crystalcontrol reagent would improve the crystal quality, and enable ZnCP to be used as a green energetic material in practical applications.In this study, the crystal-morphology and crystal-face parameters of ZnCP were simulated using the Morphology module of the Materials Studio simulation software (MS Morphology, Accelrys Corp., San Diego, CA, USA). Based on the theoretical calculations, experiments were performed to select the optimum crystal-control reagents and reaction conditions for the crystal-morphology optimization of ZnCP.