Unpredictable pandemics are likely to pose a significant global threat in the future, and biologically protective textiles will play critical roles in controlling the spread of pathogens during outbreaks. Herein, we present a novel metal–organic framework (MOF) composed of repeating units of a Cu(II)/(L-Cys)2 complex formed through coordination bonds between Cu(II) and L-Cys, while being interconnected by ionic bonds involving Cu(II) and the carboxylate group of L-Cys. After covalently embedding the MOF nanofibers onto cotton fiber surfaces, the resulting fabrics exhibit remarkable virucidal and antibacterial capabilities. Remarkably, even after 200 friction or 50 laundering cycles, the high antiviral ability to inactivate all phi- × 174 within 10 min was maintained, and the bacterial reduction rate against E. coli and S. aureus remained nearly at 100%. The remarkable virucidal effect of the L-Cys@Cu MOF structure is elucidated through a series of α-amylase denaturation simulation tests, providing the first experimental demonstration of the antiviral mechanism, whereby MOF nanofibers induce protein denaturation to inactivate viruses. Moreover, cytotoxicity assessments confirm that the fabrics adorned with MOF nanofibers are safe for human skin. These advantages are promising for the development of protective textiles, highlighting the great potential of nanoscience in combating pandemics.