Fabricating efficient materials for environmental purposes is a priority and the subject of much attention nowadays. The objectives of this study are to adopt an amino modification approach to improve the selective removal capacity of magnetic graphene oxide (MGO) for Cu(II) ions, and explore how it performs in single and binary systems by taking Cd(II) as a comparison. After grafting the amino groups, the final material exhibited promoted capacities for Cu(II) and Cd(II), and a more apparent selective adsorption process can be observed. The maximum equilibrium adsorbances of amino modified MGO were 578.1 mg g−1 for Cu(II) and 184.7 mg g−1 for Cd(II) under our experimental conditions, compared with 319.1 mg g−1 and 161.2 mg g−1 of MGO for Cu(II) and Cd(II), respectively. Characterization results and experiment data confirmed that the introduction of N species contributed to the enhancement. This may pave the way for better understanding of the underlying mechanism, and provide inspiration for synthesizing new adsorbents.