Three novel magnetic adsorbents were synthesized through the immobilization of di-, tri-, and tetraamine onto the surface of silica coated magnetite nanoparticles. The adsorbents were characterized by XRD patterns, FTIR spectroscopy, elemental and thermogravimetric analysis, magnetic measurements, SEM/TEM, EDX spectroscopy, and N2 adsorption/desorption isotherms. Their capacity to remove copper ions from aqueous solutions was investigated and discussed comparatively. The equilibrium data were analyzed using Langmuir and Freundlich isotherms. The kinetics was evaluated using the pseudo-first-order, pseudo-second-order, and intra-particle diffusion models. The best interpretation for the equilibrium data was given by the Langmuir isotherm for the tri- and tetraamine functionalized adsorbents, while for the diamine functionalized adsorbent the Freundlich model seemed to be better. The kinetic data were well fitted to the pseudo-second-order model. The overall rate of adsorption was significantly influenced by external mass transfer and intraparticle diffusion. It was observed that the adsorption capacity at room temperature decreased as the length of polyamine chain immobilized on the adsorbent surface increased, the maximum adsorption capacities being 52.3 mg g−1 for 1,3-diaminopropan functionalized adsorbent, 44.2 mg g−1 for diethylenetriamine functionalized adsorbent, and 39.2 mg g−1 for triethylenetetramine functionalized adsorbent. The sorption process proved to be highly dependent of pH. The results of the present work recommend these materials as potential candidates for copper removal from aqueous solutions.