Ca-doped magnesium oxide nanosorbent has been prepared by sol-gel in the presence of gum arabic extract and assessed for the removal of cobalt ions (Co (II)) from aqueous media. X-ray diffraction analysis indicates the formation of MgO and CaO composites with a mean crystallite size of 6 nm having a large surface area of 50 m2/g. Scanning and transmission electron microscopy observations reveal spherical-shaped particles at the nanoscale around 20 nm. Besides, X-ray photoelectron spectroscopy and Fourier transform infrared analyses manifest the existence of functional groups, which will facilitate the adsorption of metal ions. The adsorption capability of the CaO-MgO nanosorbent achieved 469.5 mg/g for Co (II) ions under optimum operating conditions. Furthermore, the experimental data elucidate that the adsorption process is primarily diffusion-based and that both intraparticle and boundary layer diffusion appear to play a key role in the rate-controlling step. The findings of this study highlight the remediation of contaminated water by cobalt ions by CaO-MgO nanostructure and can be extended to other metal ions and organic pollutants.