Caffeine, an emerging contaminant of water sources and bodies, can be removed from wastewater by clay-based adsorption, but there is a lack of tested adsorbents. In this work we created a new adsorbent material obtained from a locally available bentonite, a type of clay, from thermal treatment, and tested its variants for the removal of aqueous caffeine. The adsorbent was subject to chemical analysis and characterized using five experimental methods, while an experimental design for the effects of six variables on adsorption yield the optimal conditions for thermal treatment and application of the adsorbent. Additionally, caffeine adsorption isotherms and kinetics were obtained. The results show that aqueous caffeine removal with this new adsorbent is feasible.