For separation and regeneration of the adsorbent from aqueous solution, one spherical macro-biocomposite based on chitosan-entrapped zirconium (Chi?Zr) was synthesized, characterized, and further studied for As(V) adsorption. Various parameters including pH (1?10), initial concentration (10?100 mg L-?1), contact time (0?240?min), and temperature (4?30?C) were investigated. The results showed Chi?Zr exhibited an adsorption capacity of 190 mg g(?1) and fast kinetics toward As(V). Chi?Zr could be easily separated and regenerated, and it still kept excellent capacity after six cycles. In conclusion, Chi?Zr with fast kinetics, high-adsorption capacity, and reusability is a potential adsorbent for As(V)-contaminated wastewaters.