Silicone sponge, which is nontoxic, highly flexible, insulated, and chemically inert, has great promise in the aerospace, electronics, and health care industries. However, the inherent surface properties and the harsh synthesis method limit its application. A super‐amphiphilic 3D silicone sponge is designed by a thiol‐ene click reaction for the first time. The sponge possesses high porosity, low density, excellent adsorption ability, and reusability for water, oil, emulsions, and Hg2+ or dyes or suspended solids in them. The sponge can selectively adsorb a very high amount (941.3 mg g−1) of Hg2+ from solutions (water, oil, emulsions) containing various ions at a nearly 100% removal efficiency. Cation dyes can also be selectively captured by the sponge. Furthermore, the sponge is designed as a filter element for a filtration system, and the content of the pollutants in the filtrate reaches drinkable levels after the Hg2+ and dye solutions are processed. The filter can be reused with almost unchanged filtration efficiency after a simple washing process. The successful treatment of actual/artificial polluted water proves its practical value.