The adsorption of Ni(II) by a thermo-sensitive adsorbent of methylcellulose/calcium alginate beads (CAMCBs) was studied using batch adsorption tests to determine the adsorption process and properties, the effects of adsorbent dosage, initial concentration, adsorption time and temperature. The adsorption process was further investigated using kinetics, isotherms and thermodynamic methods. The kinetics and isotherms studies showed the adsorption of Ni(II) on CAMCBs was fitted by the pseudo-second-order kinetic model and Langmuir isothermal adsorption model, respectively. The thermodynamic parameters indicated that the adsorption process was spontaneous and exothermic at lower temperature, and the entropy of the adsorption process was negative. In the study of regeneration, it was confirmed that under the temperature of 60 °C, the desorption agent of CaCl2 with concentration of 3 g·L−1 was more conducive to the desorption of Ni(II) from CAMCBs. Both adsorption capacity and mechanical strength of the used CAMCBs could be basically recovered to the level of fresh CAMCBs after desorption. The prepared CAMCBs had a good property of adsorption of Ni(II) and an excellent regeneration performance.