Trihalomethanes (THMs) are formed during the water chlorination process through the reaction between chlorine and the organic materials. In this research, montmorillonite (MMT) and its modified form were used to remove the THMs from the water. The optimum conditions for the best adsorption capacity were evaluated using the Taguchi design of experiments. The result of comparing MMT with its modified sulfonated form (SMMT) indicated that SMMT is a more effective adsorbent than MMT. The evaluations showed that the optimum conditions for the THMs removal occur at 20 °C, 10 mg of adsorbent, 1 mg/L of THMs concentration, and 120 min for the adsorption time. The maximum adsorption capacity of CHCl3, CHBrCl2, CHBr2Cl, and CHBr3 was achieved: 0.49, 0.45, 0.43, and 0.38 mg/g at C0 = 0.10 mg/L; 1.71, 1.62, 1.56, and 1.45 mg/g at C0 = 0.50 mg/L; and 4.43, 4.35, 4.23, and 3.67 mg/g for C0 = 5.00 mg/L, respectively. The THMs adsorption was compared between SMMT, powdered activated carbon (PAC), and granular activated carbon (GAC) and the results showed that SMMT is as effective as PAC and better than GAC and its production cost is lower than for the activated carbon.