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The solubility of 2-mercapto-1,3,4-thiadiazol (MTD) in four kinds of aqueous mixed solvents including water + (methanol, ethanol, n-propanol, and acetone) was measured by the static gravimetric method in a temperature range of 278.15–323.15 K. The solubility of MTD in all selected aqueous mixed solvents was positively correlated with temperature. The solubility of MTD in the water + acetone solvent is higher than that in the other three solvents. There is a cosolvency phenomenon in the solvent systems of water + n-propanol and water + acetone. The polarity of good solvents plays an important role in the solubility of MTD in mixed solvents. Three thermodynamic models including the modified Jouyban–Acree model, NRTL model, and Wilson model were chosen to correlate the experimental data of MTD. The NRTL model fits the solubility data of MTD best among all of the selected thermodynamic models (with RAD = 0.0104, RMSD = 0.000432). The results demonstrate that all of the models can fit the experimental data well.