Recently, great efforts have been put towards developing smart textiles with desired performance and functionality, which has significance in constructing human second skin for the protection and appearance of our body.[1] Nanotechnology can extend new functions of textiles while maintaining their look and feel, showing great potential to revolutionize the medical, military, domestic, sports and clothing textiles.[2] However, previous studies mainly focused on integrating nanoparticles into textiles to gain new functionality, such as antimicrobial properties, fire retardancy, UV protection, self cleaning, sensing and human biomonitoring.[3] In addition to these excellent functionalities, clothing comfort is a fundamental and universal need for their wearer. Development of textiles with good water absorption and quick drying ability has great importance for improving clothing thermophysiological comfort and wearing performance by adjusting the transport of heat and moisture through a fabric, which was usually achieved using synthetic fibers.[4]Wool, one of the best natural insulating fibers, has an inherent deficiency in heat and moisture comfort because of the presence of a hydrophobic fatty layer that surrounds each fiber.[5] We have already developed an effective method to obtain superhydrophilic wool fabric by coating silica nanoparticles on the surface of wool, changing both surface energy and roughness of wool fabric.[6] Thanks to the silica layer's chemical stability and optical transparence, the superhydrophilic property is environment stable while the color and morphology of pristine wool fabric is unaffected. However, washing fastness is a problem because the coalesce force between the fiber and the silica nanoparticles is weak and only meets the need of dry cleaning. Although wool clothes are traditionally washed by dry cleaning, machine-washable wool clothes are a growing trend because they avoid the use of environmentally hazardous dry-cleaning solvents, and make washing easier and more convenient. Developing machine-washable wool textile and maintaining new functions endowed by nanoparticles is an important goal in the research area of the wool textile industry. There is still a great challenge to graft functional inorganic nanoparticles on the surface of wool fibers by a durable coalesce force. Therefore, developing an effective approach to enhance the coalesce force between nanoparticles and wool fibers has great significance both in scientific and real applications.We adopted a simple and effective method to functionalize reactive monolayer on wool fiber surface by chemical bonding and then graft ultrathin silica nanoparticles layer by an in situ growth method. Among the various materials used for fabrication of reactive monolayer, alkylsilane is promising for practical applications because of its marked mechanical and chemical stability, which is attributed to the strong immobilization through siloxane bonding.[7] Furthermore, the in situ growth process in this work is an effective strategy to in...