We focus on the solubility of 4-methylsulfonylacetophenone. A gravimetric method was taken to measure the solubility of 4-methylsulfonylacetophenone in n-hexane, ethyl acetate, methanol, ethanol, n-propyl alcohol, n-butyl alcohol, ethylene glycol, cyclohexane, isobutyl alcohol, and (ethyl acetate + n-hexane) binary solvent mixtures from 278.15 K to 328.15 K under atmospheric pressure. Its corresponding (solid + liquid) equilibrium results will provide essential support for further theoretical studies. The solubility of 4-methylsulfonylacetophenone in nine pure solvents were correlated with lambda h and Apelblat models, while 4-methylsulfonylacetophenone in (ethyl acetate + n-hexane) binary solvent mixtures were correlated with the Apelblat and CNIBS/R-K models. The Apelblat model was proven to be the best-fit model for correlating the solubility of both pure solvents and binary solvents mixtures from the analysis of the STATISTIC.