Hydrophobic aerogels were used to remove three types of persistent organic pollutants: pharmaceutical drugs (i.e. doxorubicin [DOX], paclitaxel [TAX]), phthalates (diethyl phthalate [DEP]), and hydrophilic rhodamine dye (RhB) from synthetic and real wastewaters, using Lumira granular aerogel from Cabot activated with EtOH (ET-GAG). The hydrophobic silica aerogel was characterized by X-ray diffraction (XRD), High-Resolution Transmission Electron Microscopy (HRTEM), Brunauer–Emmet–Teller (BET) and attenuated total reflection–Fourier transform infrared spectroscopy. The pollutants were analysed by high-performance liquid chromatography (HPLC)–UV and HPLC–mass spectrometry. The adsorption process was governed by hydrophobic- hydrophobic interactions between the ET-GAG and micropollutants. The adsorption capacity of ET-GAG, examined by batch experiments, for DOX, TAX and DEP were 13.80, 14.28 and 17.54 mg/g respectively. The rate of adsorption to ET-GAG is high in the initial 40 min followed by no change in the rate due to saturation of adsorption sites. ET-GAG was able to completely remove micropollutants from real leachate and hospital wastewater, implying practical applications. Regeneration of the aerogel was studied by solvent extraction. Et-GAG adsorbent demonstrated better removal of toxic chemotherapeutic drugs and phthalates than GAC.