An easy, comprehensive and inexpensive method is demonstrated to produce asymmetric polymer/inorganic nanocomposites in a large quantity. With the aid of Pickering emulsion, unmodified particles aggregate on the surface of emulsion droplets and are fixed in place when the wax solidifies. The exposed surfaces of immobilized SiO2 particles are modified chemically by 2-(dimethylamino) ethylmethacrylate (DMAEMA). With the removal of wax, the exposed side of particles can be further modified chemically by N-isopropylacrylamide (NIPAAm). Based on these procedures, dual responsive asymmetric nanocomposite particles are achieved with both pH and temperature sensitivities. Due to their dual-stimuli and asymmetric structure, these particles have potential applications in molecule targeting, drug delivery and as building blocks for the assembly of complex nanostructure. (C) 2012 Elsevier B. V. All rights reserved.