Four solvents (ethanol, isopropanol, ethylene glycol (EG), and N,N-dimethylformamide (DMF)) that can be mixed with water in any ratio were selected to determine the dissolution performance of 7-amino-4-methylcoumarin by the classical shake-flask method. The measured temperature range began at 278.15 K and ended at 303.15 K, and the pressure environment was controlled at standard atmospheric pressure (101.1 kPa). Results reveal that with the addition of organic solvents, the solubilization effect of 7-amino-4-methylcoumarin was very significant and the larger the amount of addition, the more obvious was the effect of solubilization. Not only that, the temperature change had a non-negligible effect on the dispersion of 7-amino-4-methylcoumarin; the temperature increased monotonically, and the better was the dissolution. When the external conditions were kept constant, the addition of DMF made the solubilization effect of 7-amino-4-methylcoumarin most obvious among all organic solvents used. This study involved three models, including the Jouyban–Acree model and its two variants (van’t Hoff–Jouyban–Acree model and Apelblat–Jouyban–Acree model), which were used to correlate the solubility data of 7-amino-4-methylcoumarin in aqueous cosolvent mixtures. The relative average deviation (RAD) and root-mean-square deviation (RMSD) reaches to 3.47 × 10–2 and 1.79 × 10–3 rooting in the van’t Hoff–Jouyban–Acree model. The relevant parameters obtained through model calculation and experimental means are essential for product synthesis, separation, and purification processes.