This study investigated the potential of 4A zeolite, named4AZW in this work, generated by natural gas dehydration units as solid waste after several treatment cycles, as a low-cost adsorbent to separately remove two cationic dyes, methylene blue (MB) and malachite green (MG), from an aqueous solution within a batch process. The adsorbent material was characterized by N₂gas adsorption–desorption, X-ray fluorescence spectrometry, X-ray diffraction, FT-IR spectroscopy, and the determination of its cation exchange capacity and point of zero charge. The influence of key operating parameters, such as the pH, adsorbent dosage, ionic strength, contact time, initial dye concentration, and temperature, was investigated. Three independent variables acting on MB adsorption performance were selected from the Box–Behnken design (BBD) and for process modeling and optimization. An analysis of variance (ANOVA), an F-test, and p-values were used to analyze the main and interaction effects. The experimental data were satisfyingly fitted with quadratic regression with adjusted R²= 0.9961. The pseudo-second-order kinetic model described the adsorption of the dyes on 4AZW. The equilibrium data were well-fitted by the Langmuir model for each adsorption system (MB-4AZW and MG-4AZW) with maximum adsorption capacity (q_max) values of 9.95 and 45.64 mg/g, respectively, at 25 °C. Thermodynamics studies showed that both adsorption systems are spontaneous and endothermic.