A carefully designed surface modification technique for the manufacture of multifunctional silk textile nanocomposite materials is successfully developed by the functionalization of silk with TiO2 and TiO2@Ag nanoparticles (NPs). The NPs are assembled onto a silk substrate through covalent linkages, including enediol ligand-metal oxide bonding, resin dehydration and the acylation of silk. Owing to the strong chemical bonding, silk fibroin fabric (SFF) and the NPs form a stable composite system. The functionalized SFF, especially TiO2@Ag NP-functionalized SFF are endowed with remarkable UV protection properties, and an efficient anti-bacterial capability toward Escherichia coli, Staphylococcus aureus, and Pseudomonas aeruginosa. Furthermore, the nearly total photodegradation of methylene orange (MO) under UV illumination illustrates that functionalized SFF possesses high photocatalytic and self-cleaning capability. This multifunctional silk material satisfies the market demand for natural "smart" products, and is a promising practical material for use in the textile industry, hospital sterilization and environmental cleanup. (C) 2011 Elsevier Inc. All rights reserved.