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Cotton fabrics with durable and reusable daylight-induced antibacterial/antiviral functions were developed by using a novel fabrication process, which employs strong electrostatic interaction between cationic cotton fibers and anionic photosensitizers. The cationic cotton contains polycationic short chains produced by a self-propagation of 2-diehtylaminoehtyl chloride (DEAE-Cl) on the surface of cotton fibers. Then, the fabric (i.e., polyDEAE@cotton) can be readily functionalized with anionic photosensitizers like rose Bengal and sodium 2-anthraquinone sulfate to produce biocidal reactive oxygen species (ROS) under light exposure and consequently provide the photo-induced biocidal functions. The biocidal properties of the photo-induced fabrics (PIFs) were demonstrated by ROS production measurements, bactericidal performance against bacteria (e.g., E coli and L. innocua), and antiviral results against T7 bacteriophage. The PIFs achieved 99.9999% (6 log) reductions against bacteria and the bacteriophage within 60 min of daylight exposure. Moreover, the PIFs showcase excellent washability and photostability, making them ideal materials for reusable face masks and protective suits with improved biological protections compared with traditional PPE. This work demonstrated that the cationized cotton could serve as a platform for different functionalization applications, and the resulting fiber materials could inspire the development of reusable and sustainable PPE with significant bioprotective properties to fight the COVID-19 pandemic as well as the spread of other contagious diseases.