The solubility of pyrimethanil in two binary solvents (water + methanol and water + ethanol) and seven monosolvents (methanol, ethanol, n-propanol, isopropanol, n-butanol, isobutanol, and cyclohexane) was measured by a gravimetric method within the temperature range of 283.15 to 323.15 K at atmospheric pressure. In the investigated temperature range, the solubility of pyrimethanil in all monosolvents or mixed solvents increases with increasing temperature. The solubility in the monosolvents was well correlated using the NRTL model, the Apelblat model, and the Wilson model. Furthermore, the NRTL model and the modified version of the Jouyban-Acree model (the Apel-JA equation) were employed to correlate the solubility in binary solvents. The results showed that these models have a satisfactory correlation. When we measured the solubility, we found that the solvent has a great influence on the crystal habit. Therefore, these results can give guidance for practical industrial processes such as the design of the crystallization process and control of the crystal morphology.