Vermiculite clays are adsorbent materials that have good chemical adsorption capacity, which makes them applicable in the removal of drugs from aqueous solutions. Their lamellar structure can be easily expanded and organophilized. To assess the efficacy and environmentally-tolerant capacity of the adsorption method, the organophilized vermiculite clay was compared to both natural and expanded vermiculite clays. To prepare the organophilized clays, a natural clay sample was expanded at 900 °C. The expanded clay was thus treated by immersion in a 1.0 M NaCl solution and organophilized using a cetyltrimethylammonium bromide (CTMA-Br) surfactant, for 24 h at 50 °C. Natural, expanded, and organophilized samples were characterized using the techniques of XRD, FTIR, TG/DSC, and SEM to observe structural changes after expansion and organophilization. These characterizations indicated that there was an increase in the interlamellar space of the expanded and organophilized sample. In addition, a study of the point of zero charge was performed to determine the surface changes of the samples and the amount of doxazosin adsorption in the samples was determined by the time adsorption test. Further, the organophilized sample showed potential adsorption of the drug doxazosin and high performance in relation to the expanded and natural samples.