We report the application of Fe 3 O 4 -functionalized boron nitride nanosheets (BNNS-Fe 3 O 4 nanocomposite) for the remediation of As(III) ions from contaminated water. The specific surface area of the nanocomposite has been found as 179.5 m 2 g −1 .Due to its superparamagnetic nature at room temperature, the nanocomposite can be easily isolated from the solution under an external magnetic field. For As(III) ions, the maximum adsorption capacity of the nanocomposite is obtained as 30.3 mg g −1 , which is approximately 4 times more than that of the bare BNNSs (8.5 mg g −1 ). The results from density functional theory calculations are also in close agreement with experimental findings and show that As(OH) 3 binds more (∼4 times) efficiently to the BNNS-Fe 3 O 4 nanocomposite than the bare BNNSs, implying a 4 times higher adsorption capacity of the nanocomposite. Especially, it is found that the synthesized nanocomposite could lessen the concentration of As(III) ions from 134 to 2.67 ppb in a solution at 25 °C. On increasing the temperature to 35 °C, the level of As(III) ions could be reduced from 556 to 10.29 ppb, which is close to the limit prescribed by the World Health Organization. The adsorbent was easily separable and showed regeneration properties. These outcomes depict the prospect of using BNNS-Fe 3 O 4 nanocomposites as commercial adsorbents for the removal of As(III) ions from contaminated water.