Porous alginate-based hydrogel beads (porous ABH) have been prepared through a facile and sustainable template-assisted method using nano-calcium carbonate and nano-CaCO3 as pore-directing agent for the efficient capture of methylene blue (MB). The materials were characterized by various techniques. The sorption capacities of ABH towards MB were compared with pure sodium alginate (ABH-1:0) in batch and fixed-bed column adsorption studies. The obtained adsorbent (ABH-1:3) has a higher BET surface area and a smaller average pore diameter. The maximum adsorption capacity of ABH-1:3 obtained from Langmuir model was as high as 1,426.0mg g?1. The kinetics strictly followed pseudo-second order rate equation and the adsorption reaction was effectively facilitated, approximately 50minutes to achieve adsorption equilibrium, which was significantly shorter than that of ABH-1:0. The thermodynamic parameters revealed that the adsorption was spontaneous and exothermic. Thomas model fitted well with the breakthrough curves and could describe the dynamic behavior of the column. More significantly, the uptake capacity of ABH-1:3 was still higher than 75% of the maximum adsorption capacity even after ten cycles, indicating that this novel adsorbent can be a promising adsorptive material for removal of MB from aqueous solution under batch and continuous systems.