Inspired by the silica formation process mediated by silica deposition vesicle (SDV) in diatoms or sponges, silica nanoparticles (SiO2) were in-situ formed within oleophilic polydimethylsiloxane (PDMS) bulk matrix through the controlled biomimetic mineralization in confined space, using either NH3 or cysteamine as inducer/catalyst. Accordingly, different kinds of PDMS-SiO2 nanocomposite membranes were fabricated. It was observed that alkaline/basic inducers and silicon precursors with higher reactivities were more favorable for tailoring the free volume property of the nanocomposite membranes, rendering the dramatic enhancement of mechanical strength and pervaporation separation performance. The as-prepared membrane displayed an optimum desulfurization performance with permeation flux of 7.36 kg/(m(2)h) and the selectivity of 4.98 towards thiophene in model gasoline. (c) 2012 Elsevier B.V. All rights reserved.