The boron removal capacity from an aqueous solution using MgAlFe mixed oxides from layered double hydroxides (LDH) was studied. They were synthesized by the coprecipitation method at 70 °C and were characterized as potential filter materials. The Fe3+ analyzed by X-ray photoelectron spectroscopy and UV–visible diffuse reflectance showed their tetrahedral and octahedral coordination. Scanning electron microscopy micrographs and thermogravimetric and differential scanning calorimetry analysis evidenced the presence of clusters and particles aggregates and decreased dehydroxylation temperature when the iron content increased. Mixed oxides and boron solution in a ratio of 20:1 Mg/B were put in a batch reactor at different contact times. The borate removal process was due to the memory effect of the mixed oxides and superficial adsorption by electrostatic attraction. This fact is directly related to the specific surface area, Fe content, and surface charge. The maximum boron removals were achieved with the CS25 and CS50 samples with values higher than 85%.