In this study, a new pleated hollow sphere material (CS@Ca@CTA) was prepared by mixing chitosan (CS) and calcium chloride (CaCl2) in acetic acid solutions followed by crosslinking with glutaraldehyde (GA), and quaternized using (3-chloro-2 hydroxypropyl) trimethylammonium chloride (CTA). The natural biopolymer chitosan (CS) was used to prepare an environmentally friendly adsorbent material which can efficiently adsorb sodium dodecylbenzene sulfonate (SDBS). The adsorption of SDBS on CS@Ca@CTA can be efficiently improved by CTA at different pH values and Ca can promote the precipitation. The adsorption process of SDBS is as follows. First, SDBS can be adsorbed by electrostatic attraction and Cl-of CTA is used to ion exchange DBS of SDBS. Then DBS- can bind stably with the Ca2+ in a bidentate form. Furthermore, CS contains NH2 and OH groups, which can provide enormous vacant active sites to adsorb SDBS, and a pleated surface have an ability to capture SDBS. The results indicated that the saturated adsorption capacity of CS@Ca@CTA up to 2300 mg g-1 at pH 3.0 within 240 min. Additionally, adsorption kinetics, isotherm and thermodynamic parameters were discussed. The aim of this article is to present CS@Ca@CTA, which has a great effect on adsorbing the SDBS.