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Ion desorption is extremely challenging for adsorbents with superior performance, and widely used conventional desorption methods involve high acid or base concentrations and large consumption of reagents. Here, we experimentally demonstrate the rapid and efficient desorption of ions on magnetite-graphene oxide (M-GO) by adding low amounts of Al3+. The corresponding concentration of Al3+ used is reduced by at least a factor 250 compared to conventional desorption method. The desorption rate reaches ~97.0% for the typical radioactive and bivalent ions Co2+, Mn2+, and Sr2+ within ~1 min. We achieve effective enrichment of radioactive 60Co and reduce the volume of concentrated 60Co solution by approximately 10 times compared to the initial solution. The M-GO can be recycled and reused easily without compromising its adsorption efficiency and magnetic performance, based on the unique hydration anionic species of Al3+ under alkaline conditions. Density functional theory calculations show that the interaction of graphene with Al3+ is stronger than with divalent ions, and that the adsorption probability of Al3+ is superior than that of Co2+, Mn2+, and Sr2+ ions. This suggests that the proposed method could be used to enrich a wider range of ions in the fields of energy, biology, environmental technology, and materials science. Desorption of ions from sorbents generally involves high acid or base concentrations and long desorption times, especially for multivalent ions. Here the authors report a rapid and efficient desorption of Co2+, Mn2+, and Sr2+ adsorbed on magnetite-graphene oxide that occurs by adding low amounts of Al3+, which is shown to interact with graphene more strongly than divalent ions. [ABSTRACT FROM AUTHOR]