In this paper, we focused on the solubility of phenylbutazone, which was characterized by FT-IR spectra and X-ray diffraction. By the method of a laser technique, the solubility of phenylbutazone was measured in 10 monosolvents (methanol, ethanol, 2-propanol, n-butanol, 1-pentanol, n-hexanol, acetonitrile, ethyl acetate, acetone, and DMF) and 2 binary solvent mixtures of methanol + acetone and ethanol + acetonitrile from 283 to 323 K at about 5 K intervals under atmospheric pressure. The results show that the solubility of phenylbutazone in monosolvents and mixed solvents increases with the increase of temperature. However, it decreases with the increasing initial mole fraction of alcohols in the selected mixed solvents at constant temperature. The experimental data were correlated by the modified three-parameter van't Hoff equation and the modified Jouyban-Acree equation.