The organo-attapulgite was prepared using hexadecyltrimethylammonium bromide (HTMAB) with equation equivalent ratio of HTMAB to CEC of attapulgite added and then used as adsorbent for the removal of Congo red (CR) anionic dye from aqueous solution. Adsorbent characterizations were investigated using infrared spectroscopy and X-ray diffraction. The effects of contact time, temperature, pH and initial dye concentration on organo-attapulgite adsorption for CR were investigated. The results show that the amount adsorbed of CR on the organo-attapulgite increase with increasing dye concentration, temperature, and by decreasing pH. The adsorption kinetics was studied with the pseudo-first-order, pseudo-second-order and intraparticle diffusion models, and the rate constants were evaluated. It was found that the adsorption mechanisms in the dye/organo-attapulgite system follow pseudo-second-order kinetics with a significant contribution of film diffusion. Equilibrium data fitted perfectly with Langmuir isotherm model compared to Freundlich isotherm model, and the maximum adsorption capacity was 189.39 mg g −1 for the adsorbent. Kinetic and desorption studies both suggest that chemisorption should be the major mode of CR removal by the organo-attapulgite. The results indicate that HTMABmodified attapulgite could be employed as low-cost material for the removal of Congo red anionic dye from wastewater.