Very little attention has been focused on the purifi cation of water-soluble pollutants after oil/water separation. [ 4 ] Thus, there is considerable interest in developing novel and facile methods for the simultaneous separation of oil from water and purifi cation of water-soluble pollutants.The practical application of organic micelle catalysts that utilize hydrophilic/ hydrophobic interfaces has been limited by several disadvantages. For example, the stability of organic micelles depends on many parameters, such as the solvent polarity, critical micelle concentration, and reaction conditions, such as pH, water/oil ratio, and temperature. [ 10,11 ] Due to the narrow range of stability of organic micelles, the synthesis of inorganic micelles that have hydrophilic/hydrophobic interfaces, large surface areas, high porosities, tunable surfaces, and high recyclability has recently attracted some attention. [ 12,13 ] For example, Lin and co-workers reported a simple route to hierarchically assembling micelles and inorganic nanoparticles. [ 14 ] Yang and co-workers prepared functionalized mesoporous silica spheres consisting of a hydrophobic core and a hydrophilic micellar shell. [ 15 ] As a fi rst example, Alivisatos and co-workers recently reported resin templates based on the synthesis of inorganic micelles with a hydrophilic cavity and a hydrophobic surface and its application as a catalyst in the bromination of alcohol. [ 16 ] There is still considerable interest in developing novel methods for the exploration of interior/ exterior-functionalized, superhydrophobic, and nanostructured inorganic micelles. To fulfi ll the requirements of oil/water separation and inorganic micellar catalysis mentioned above, the development of hierarchical nanomaterials that have a hydrophilic interior and superhydrophobic/hydrophilic (amphiprotic) exterior is highly desirable, offering signifi cant potential for multiple applications. To the best of our knowledge, this report is the fi rst example of the synthesis of nanomaterials that have a hydrophilic core and amphiprotic shell for multiple applications, such as amphiprotic catalytic reactions, oil/water separation and pollutant purifi cation, and enzyme immobilization with signifi cant stability and effi cient recyclability.Herein, we present the preparation and multiple applications of superhydrophobic hollow SiO 2 micelles (SHSMs) with hydrophilic cores and amphiprotic (superhydrophobic/hydrophilic) shell structures that act as "all-in-one" smart nanomaterials. Our SHSMs are better than hydrophilic@hydrophobic micelles prepared using previously reported methods for several reasons: (i) the polyallylamine hydrochloride (PAH) chains were extended and survived from the core to the shell even Inorganic Micelles (Hydrophilic Core@Amphiprotic Shell) for Multiple Applications Md. Shahinul Islam , Won San Choi , * Sun Ha Kim , Oc Hee Han , and Ha-Jin Lee * A facile approach for synthesizing superhydrophobic hollow silica micelles (SHSMs) with hydrophilic cores and amphiprotic (supe...