Perfluorooctanoic acid (PFOA) and perfluorooctanesulfonic acid (PFOS) as the two most typical perfluorinated compounds, their effective and rapid removal are still facing enormous challenges. In this study, the adsorption performance and mechanism of PFOA and PFOS by ball milled micrometer zero valent magnesium (mZVMg) were revealed firstly through the adsorption kinetics and isothermal, ions coexisting competitive adsorption and extraction experiments. Rapid adsorption equilibrium within 0.5 h was observed in the mZVMg system, and the higher adsorption affinities at 1.9 and 6.5 L/mg for PFOA and PFOS respectively were approximately 4.4–110 times higher than those of the carbon materials, layered double hydroxide and magnetite reported in the literature. Correspondingly, high removal efficiencies for PFOS were observed even under a wide pH ranging from 3.0 to 11.0. In the meantime, negligible influences on the PFOS adsorption were identified from the coexisting PFOA, perfluorobutanoic acid (PFBA), perfluorobutanoic sulfonic acid (PFBS), anions of Cl−, NO3− and SO42−. Reversely, the PFOA adsorption was adversely influenced by enhanced electrostatic repulsion under the increased pH and the presence of the abovementioned anions. Additionally, the original removal efficiency of 67.18 % for PFOA in the absence of any cations and anions was decreased to 7.98 %, 31.08 % and 39.65 % respectively in the presence of humic acid, HCO3− and CO32−. Similarly, the removal efficiency of 94.41 % for PFOS was declined to 40.01 %, 70.04 % and 80.58 % respectively when humic acid, HCO3− and CO32− were added to the solution. However, in the presence of respective Mg2+ and Ca2+, the original removal efficiencies were increased from 67.18 % to 75.78 % and 74.68 % for PFOA, and from 84.99 % to 93.23 % and 92.49 % for PFOS, likely due to the cation’s bridge effect. Consequently, the hydrophobic adsorption and electrostatic interaction accounted for 71.3 % and 19.75 % for PFOA, while 86.26 % and 5.85 % for PFOS removal, respectively through the solvent extraction and long-term effective removal experiments. Overall, this study provided an alternative, promising and environmental-friendly mZVMg for rapid adsorption of PFOA and PFOS.