Results of the interaction of process variables and the consequential mixture of phenolic compounds adsorption study are expected to shed brighter light on the wastewater treatment applications. Accordingly, the aims of this research are to model and optimize the process variables which impinged on the simultaneous adsorption of phenol and 4-chlorophenol (4-CP) in the binary solution by spherical activated carbon (SAC). Batch assessments were designed using response surface methodology software. The process variables, namely SAC dosage and pH were varied over the 1.50�3.50 g/L and 4.00�9.00 g/L ranges, respectively, were experimented. The analysis of variance results showed the significant models could precisely predict the percentage removals of phenol and 4-CP, indicating models reliability. The interaction of process variables was inconspicuous for the case of phenol adsorption. However, increasing the pH would deteriorate the 4-CP adsorption which was partially offset by raising the SAC dosage. Considering the environmental benefits, optimization taken place at the SAC dosage and pH of 3.50 g/L and 7.60 g/L, respectively, was selected. By employing the optimized conditions of SAC dosage of 3.50 g/L at pH 7.60 for the adsorption process, the predicted phenol and 4-CP removal percentages were found to be 85.4 (73.1 mg/g) and 96.2 (82.6 mg/g), respectively, which were in agreement with the experimental runs. © 2016, The Author(s).