We report the bioassisted synthesis of gold nanoparticle/silica (Au NP/silica) tubes using layer-by-layer (LBL) assembled poly(L-lysine)/poly(L-tyrosine) (PLL/PLT) multilayer films deposited on the polycarbonate (PC) membrane pores as both mediating agents and templates. The novelty of this approach is the in situ synthesis of Au NP/silica tubes using PLL/PLT multilayer films for sequential growth of Au NPs and silicas. The experimental data revealed that the buildup of the LBL multilayer films was mainly driven by the formation of hydrogen bond and the polypeptide macromolecular assemblies adopted mainly beta-sheet conformation. The as-prepared Au NP/silica tubes possessed promising catalytic activity toward the reduction of p-nitrophenol. The synthesis conditions such as the concentration of gold precursor and polypeptide molecular weight were found to influence the gold weight ratio and particle size in the tubes and the catalytic properties of the Au NP/silica tubes. This approach provides a facile, robust, and green method to obtain nonaggregated metal nanoparticles immobilized in porous oxide network at ambient conditions. Using the synergy between biomimetic or bioassisted synthesis of nanostructured materials and LbL assembly technique, a variety of structures such as films, tubes, and capsules comprising of multiple compositions can be obtained. (C) 2011 Elsevier Inc. All rights reserved.