The synthetic imogolite sample was used for organofunctionalization process with 2-mercaptothiazoline (MTZ). The compound 2-mercaptothiazoline was anchored onto imogolite surface by heterogeneous route. Due to the increment of basic centers attached to the pendant chains the dye adsorption capability of the final chelating material, was found to be higher than is precursor. The ability of these materials to remove methylene blue from aqueous solution was followed by a series of adsorption isotherms at room temperature and pH 4.0. The maximum number of moles adsorbed was determined to be 40.32 x 10(-2) and 65.13 x 10(-2) mmol g(-1) for IMO and IMOMTZ, respectively. The energetic effects caused by dye cations adsorption were determined through calorimetric titrations. Thermodynamics indicated the existence of favorable conditions for such methylene blue-nitrogen and sulfur interactions. (C) 2010 Published by Elsevier B.V.