Water contaminated with toxic dyes poses serious problems for human health and environmental ecosystems. Unfixed reactive dyes and their hydrolyzed form are soluble in water, thus, their removal is particularly challenging. Among the different methodologies, adsorption is probably the most common since it is easy to handle and has a low cost. Here, the removal by adsorption of hydrolyzed Reactive Black 5 (hydRB5) from a model wastewater through cellulose acetate/hematite membranes (CA/α-Fe2O3), designated as M1, M2 and M3, was performed. The pristine cellulose acetate membrane (CA) was designated as M0. Toward understanding the adsorption mechanism of hydRB5 on membranes, the rate of adsorption and maximum value of the adsorption capacity were evaluated using kinetic and isothermal studies, respectively. The results showed that the adsorption mechanism follows pseudo-first-order kinetics, and data are best fitted by the Langmuir isotherm method with a maximum adsorption capacity of 105.26 mg g−1 in pH~7. Furthermore, these membranes can be also regenerated by washing with NaOH and NaCl solutions, and the regeneration efficiency remains effective over five cycles. To complete the work, two statistical models were applied, an Analysis of Variance (ANOVA) and a Response Surface Methodology (RSM). The optimum value found is located in the usable region, and the experimental validation shows good agreement between the predicted optimum values and the experimental data. These composite membranes are also good candidates for the adsorption of other pollutants, even at industrial scale, due to their effective regeneration process and low production costs.