Since arsenic is highly toxic and carcinogenic, it now causes serious health problems all over the world. Therefore, there is an urgent need to develop new techniques that are cost-effective and easily applicable to remove arsenic from contaminated waters. Layer double hydroxides have the potential to be a good adsorbent to remove arsenic from contaminated waters due to high surface area and high anion exchange capacity. In this paper, arsenic removal from water by calcined Fe-hydrotalcite (CFeHT) known as layered double hydroxide and prepared synthetically with coprecipitation method was researched. The study brings out that the effect of initial solution pH values was limited for the adsorption. The experimental study indicates that the adsorption of arsenic rapidly occured in comparison with other studies. It was determined that the pseudo-second-order kinetic model was more suitable than the first order. In isotherm studies, it was seen that the experimental data were compatible with Langmuir model. In this study was determined that CFeHT has a high arsenic removal potential. And also the concentration of the arsenic solution (600 µg/L) has been reduced below the allowable value by the World Health Organization (< 10 µg/L). The desorption test indicates that the desorption ratio of As(V) was obtained as 72.7.