Development of a novel strategy to tackle bacterial-contaminated complex industrial wastewaters containing refractory organic pollutants is of great demand. In this study, polydopamine (PDA)-coated magnetic cellulose nanofiber (MCNF)-loaded silver nanoparticle (AgNP) (MCNF/PDA-Ag) nanocomposites were designed and applied for efficient degradation of organic dye pollutants and inactivation of Escherichia coli (E. coli) in wastewater. In the presence of NaBH4, MCNF/PDA-Ag could achieve a high catalytic reduction rate of 6.54 min-1 for the removal of methylene blue. Similarly, it showed good catalytic reduction performance for methyl orange (0.63 min-1) and 4-nitrophenol (2.94 min-1). The MCNF/PDA-Ag nanocomposites can be easily magnetically recycled and reused with negligible loss of catalytic performance. Moreover, this nanocatalyst also exhibited excellent disinfection performance against E. coli, with more than 99% disinfection ratio at very low doses (50 μg/mL). Overall, this work provides new insights into a delicate design of advanced magnetically recyclable silver nanocomposites with ultrahigh catalytic rates and excellent antibacterial properties from sustainable nature biomass.