There is a critical need for new efficient solutions to purify and disinfect water from source to point-of-use, especially for the water contaminated by pathogenic microbes. Traditional disinfection technologies are chemically intensive and limited, either by biofouling or by the irreversible consumption of disinfectants. Herein, we present a scalable methodology to create biocidal and rechargeable nanofibrous membranes (BNF membranes) by combining N-halamine antimicrobial agent with electrospun nanofibers. Our method allows intrinsically rechargeable N-halamine moieties to covalently incorporate into nanofibers with high biocidal activity and durability. The resulting BNF membranes exhibit integrated properties of high porosity, large surface area, robust mechanical strength, super hydrophilicity, rechargeable chlorination capability (>3000 ppm), and high bactericidal efficacy (99.9999% contact-killing), which enabled the BNF membranes effectively disinfect bacteria-contained water by direct filtration, with promising high durability and fluxes (10000 L m(-2) h(-1)). The successful synthesis of BNF membranes also provides a versatile platform for exploring the antimicrobial N-halamine materials in a self-supporting, structurally adaptive, and nanofibrous form.