The use of multifunctional finishing methods, in which chemical agents are applied in a combined bath or a single step to impart specific functional properties to textiles, is becoming increasingly popular. However, the existing finishing methods cannot satisfy the requirements of green and sustainable development; specifically, such methods employ materials that are toxic to humans, consume a large number of chemicals and energy, generate harmful liquid waste, and rely on expensive equipment and complex operation processes, among other factors. This paper proposes a novel and ecofriendly approach involving engineered water nanostructures (EWNSs), based on the mechanism of electrospraying and the ionization of water. EWNSs exhibit unique physical and biological properties, such as an extended lifespan, high reactivity [because of the generation of reactive oxygen species (ROS)], and strong surface charge. The ROS wrapped in EWNSs, primarily including hydroxyl (OH • ) and superoxide radicals (O 2•− ), are highly active and react easily with certain materials, thereby modifying the surface properties of textiles by forming new functional groups on the material surface or changing the surface structures of the fibers. The proposed EWNS technology is consistently effective in improving the antibacterial activity, wetting ability, and pilling resistance of cotton, polyester, and wool, while ensuring the mechanical and esthetic properties of these materials. Moreover, this facile and versatile method utilizes a limited amount of water, leaves no chemical byproducts, and does not pose a risk to human health, thereby making it an appealing multifunctional finishing method that can be applied in various fields.