A new one-pot redox route has been developed for simultaneous syntheses of Ag nanoparticles on MoO3 nanofibers. Four different synthetic reactions that have been integrated into the one-pot synthesis include the oxidation of [Na(H2O)(2)](0.25)MoO3 bronze, the reduction of silver ions, and the in situ simultaneous growth of the self-organized Ag nanoparticles and the MoO3 nanofibers. This new strategy can be generally applicable to grafting various metal nanoparticles on nanofibers for new catalysis-related applications.