The experimental gramine solubilities in pure organic monosolvents containing methanol, ethanol, n-propanol, isopropanol, n-butanol, acetone, toluene, acetonitrile, ethyl acetate, 1,4-dioxane, n-octanol, and binary solvent mixtures (ethanol + ethyl acetate) were determined by means of the isothermal equilibrium method at evaluated temperatures from (273.15 to 313.15) K under a pressure of 101.2 kPa. The solubility of gramine in neat solvents rose with rising temperature. The solubility data of gramine from high to small in the selected solvents was as follows: 1,4-dioxane > n-butanol > n-propanol > methanol > acetone > ethanol > ethyl acetate > isopropanol > n-octanol > acetonitrile > toluene. As for the (ethanol + ethyl acetate) mixture, the largest solubility was found in w(ethanol) = 0.6 at 313.15 K Differential scanning calorimetry analysis was employed, showing that the gramine's fusing point in terms of recrystallization crystals from the beginning to end in the studied solvent systems hardly changed, resulting in no crystal change during the recrystallization process. The solubility data of gramine in various monosolvents were correlated and calculated via the modified Apelblat equation, lambda h equation, NRTL equation, and Wilson equation and those of the binary solvent systems utilizing the Jouyban-Acree model, modified Apelblat-Jouyban-Acree model, and van't Hoff-Jouyban-Acree model. Results show that the maximum RAD and RMSD were 4.22% and 1.71 x 10(-3), respectively.