In this research, response surface methodology (RSM) approach using Central Composite Design (CCD) coupled by derivative spectrophotometry method was applied to develop mathematical model and optimize process parameters for simultaneous adsorption of methylene blue (MB) and malachite green (MG) from aqueous solution using Ni:FeO(OH)‐NWs‐AC. The optimal conditions to adsorption of MB and MG in binary mixture solution from aqueous solution were found at pH 8.0, MB concentration 20 mg L‐1, MG concentration 20 mg L‐1, adsorbent dosage 0.033 g and contact time 40 min. At these conditions, high adsorption efficiency (99.39% and 100.0% for MB and MG, respectively) was achieved. Among experimental equilibrium, Langmuir isotherm model fitted well with maximum monolayer adsorption capacity of 28.6 and 29.8 mg g‐1 for MB and MG, respectively. The adsorption kinetic data followed pseudo second‐order kinetics for MB and MG dyes.