In the present research, treatment of contaminated groundwater via adsorption of As(V) with an initial concentration of 50.99 µg/L using chitosan-coated bentonite (CCB) was investigated. The effect of adsorbent mass (0.001 to 2.0 g), temperature (298 to 328 K), and contact time (1 to 180 min) on the removal efficiency was examined. Adsorption data was evaluated using isotherm models such as Langmuir, Freundlich, and Dubinin-Radushkevich. Isotherm study showed that the Langmuir (R2 > 0.9899; χ2 ≤ 0.91; RMSE ≤ 4.87) model best correlates with the experimental data. Kinetics studies revealed that pseudo-second order equation adequately describes the experimental data (R2 ≥ 0.9951; χ2 ≤ 0.8.33; RMSE ≤ 4.31) where equilibrium was attained after 60 min. Thermodynamics study shows that the As(V) adsorption is non-spontaneous (ΔG0 ≥ 0) and endothermic (ΔH0 = 8.31 J/mol) that would result in an increase in randomness (ΔS0 = 29.10 kJ/mol•K) within the CCB-solution interface. FT-IR analysis reveals that hydroxyl and amino groups are involved in the adsorption of As(V) from groundwater. Results of the present research serve as a tool to determine whether CCB is an environmentally safe and cost effective material that could be utilized in a permeable reactive barrier system for the remediation of As(V) from contaminated groundwater.