The morphologies of homoharringtonine were conveniently controlled by solvent treatment and the morphologies of homoharringtonine were characterized by XRD and SEM. Crystalline homoharringtonine was simply made by dissolving homoharringtonine in a special polar solvent containing a small amount of water (methanol/water=98/2, v/v). On the other hand, amorphous homoharringtonine was made by dissolving homoharringtonine in relatively non-polar solvent (methylene chloride/methanol=98/2, v/v). Amorphous homoharringtonine, with a fine particle size, was obtained by dissolving in methylene chloride/methanol (98/2, v/v), following by spray drying. Also, residual solvents, methanol and methylene chloride, were easily removed to less than concentration limit in ICH (International Conference on Harmonisation) guidance by spray drying and successive drying in a vacuum oven. Amorphous homoharringtonine was more soluble in water than crystalline homoharringtonine, and the water content of amorphous homoharringtonine was less changeable than crystalline homoharringtonine at given humidity (95 RH%) during storage. This information is very useful for production and quality control of pharmaceuticals in the commercialization step.