Using sodium alginate hydrogel as skeleton, in combination with chitosan and magnetic FeO, a new type of magnetic chitosan/sodium alginate gel bead (MCSB) was prepared. Adsorptive removal of Cu(II) from aqueous solutions was studied by using the MCSB as a promising candidate in environmental application. Different kinetics and isotherm models were employed to investigate the adsorption process. Based on Fourier transform infrared spectroscopy, field-emission scanning electron microscope, CHNS/O elements analysis, vibration magnetometer, and various means of characterization, a comprehensive analysis of the adsorption mechanism was conducted. The MCSB had a good magnetic performance with a saturation magnetization of 12.5 emu/g. Elemental analysis proved that the addition of chitosan introduced a considerable amount of nitrogen-rich groups, contributing significantly to copper adsorption onto gel beads. The contact time necessary for adsorption was optimized at 120 min to achieve equilibrium. Experimental data showed that the adsorption process agreed well with the Langmuir isotherm model and the pseudo-second-order kinetics model. The theoretical maximum adsorption capacity of MCSB for Cu(II) could reach as high as 124.53 mg/g. In conclusion, the MCSB in this study is a novel and promising composite adsorbent, which can be applied for practical applications in due course.