Heavy-metal sources in urban environments include automobile exhaust, fuel combustion, tires, road asphalt, weathering of building materials, and/or industrial activities. The presence of heavy metals in urban stormwaters constitutes a potential risk for water resources and aquatic life. Results from the present study demonstrated the effectiveness of two different lightweight aggregates (LWAs), Arlita and Filtralite, to remove heavy metals (Ni, Cu, Zn, Cd, and Pb) present in aqueous solutions. These materials were selected because they previously showed great results for water treatment and because of their physicochemical properties. The removal efficiency of the studied materials was evaluated with batch tests containing solutions contaminated with heavy metals (with individual and multiple contaminants) at different concentrations mixed with the LWA particles. Filtralite showed a better performance in heavy metal removal than Arlita: higher adsorption capacity for all metals, and lower release of metals from contaminated particles into washing water. The average removal capacities in tests developed with solutions containing individual contaminants for Arlita and Filtralite were 76% and 90%, respectively, although the values varied across the different contaminants. Metal elimination by LWAs was more effective with individual contaminated solutions than with multielemental ones. The analysis of the adsorption curves, the mineral precipitation on the LWA surface, and the geochemical modeling confirmed that two different mechanisms are responsible for the heavy-metal removal. First, the rough surface of the LWA presents sorbing surface sites of the forming minerals, resulting in the ion-exchange reactions of metal ions. Second, the LWA–water interaction causes an increase in solution pH, which triggers the precipitation and coprecipitation of the metals in the form of oxide and hydroxides. The study confirms that the use of Arlita and especially Filtralite present promising potential to remove heavy metals from urban stormwaters.