This study aimed to develop magnetic Fe3O4/sugarcane bagasse activated carbon composite for the adsorption of arsenic (III) from aqueous solutions. Activated carbon (AC) was prepared from sugarcane bagasse by chemical activation using H3PO4 as an activating agent at 400 °C. To enhance adsorption capacity for arsenic, the resultant AC was composited with Fe3O4 particles by facile one-pot hydrothermal treatment. This method involves mixing the AC with aqueous solution of iron (II) chloride tetrahydrate, polyvinyl pyrrolidone (PVP), and ethanol. Batch adsorption experiments were conducted for the adsorption of As (III) onto the composite. The effects of pH, adsorbent dosage, and contact time on the arsenic adsorption were studied. The result showed that the composite could remove the arsenic from the water far more effectively than the plain AC. The highest percentage of arsenic removal was found at pH at 8, adsorbent dose of 1.8 g/L, and contact time of 60 min. Langmuir and Freundlich adsorption isotherm was used to analyze the equilibrium experimental data. Langmuir model showed the best fit compared to the Freundlich model with a maximal capacity of 6.69 mg/g. These findings indicated that magnetic Fe3O4/sugarcane bagasse AC composite could be potentially applied for adsorptive removal of arsenic (III) from aqueous solutions.