The energy industry (nuclear, battery, mining industries, etc.) produces a large quantity of hazardous effluents that may contain radionuclides (137Cs and 90Sr in particular) and heavy metals. One of the hardest tasks of environmental safety and sustainable development is the purification of wastewater holding these pollutants. Adsorption is one of the most powerful methods for extracting toxic compounds from wastewater. This study reviews the usefulness of clay minerals as adsorbent for removing these hazardous elements to clean up energy production processes. Phyllosilicates are able to extract several heavy metals from effluent, as widely examined. A particular focus is given to synthetic phyllosilicates and their abilities to entrap heavy metals with a special attention paid to those synthesized by sol-gel route. Indeed, this method is attractive since it allows the development of organic–inorganic hybrids from organosilanes presenting various functions (amino, thiol, etc.) that can interact with pollutants. Regarding these pollutants, a part of this review focuses on the interaction of lamellar materials (natural and synthetic phyllosilicates as well as layered double hydroxide) with heavy metals and another part deals with the adsorption of specific radionuclides, cesium and strontium.