In this work, activated carbon (AC) coated by chitosan was synthesized and characterized by Fourier transform infrared spectrophotometer and scanning electron microscope (SEM) techniques. The removal of aniline from aqueous solutions by AC coated by chitosan was investigated. The factors affecting the adsorption of aniline onto AC coated by chitosan, including the ratio of AC to chitosan, adsorbent dosage, pH value of solution, initial aniline concentration, and contact time were evaluated. These results showed that the optimum operating conditions were: the ratio of AC to chitosan = 0.5, adsorbent dosage = 0.2 g, and the adsorption of aniline from aqueous solutions had better removal in the concentration range of 20–50 mg/L. This adsorbent allowed high removal toward aniline in a wide range of pH. The equilibrium time was 100 minutes. The Freundlich model exhibited better correlation of the equilibrium adsorption data. The pseudo-second-order kinetic equation could better describe the kinetic behavior of aniline adsorption.