The recovery of uranium from seawater by adsorption is strategically important for the sustainability of nuclear energy. However, marine biofouling reduces the adsorption efficiency in adsorbents of uranium-(VI) ions. To develop biomass adsorbents with good adsorption capacity and antibiofouling properties, we propose a strategy to release free thiol groups by cleaving the disulfide bonds in wools and then via thiol-ene click reaction and in situ coprecipitation, preparing Ag-loaded amidoxime-functionalized wool fibers (Ag@Wool-AO) for selective adsorption of U-(VI) ions. The prepared adsorbents were characterized by Fourier transform infrared spectroscopy, scanning electron microscopy, energy-dispersive spectroscopy, and X-ray photoelectron spectroscopy. The adsorption properties, selectivity, antibacterial properties, and reusability of Ag@Wool-AO as an adsorbent of U-(VI) ions were also studied. The results showed that while the adsorption process was at 25 degrees C and pH 6.0 with the initial concentration of uranium ions at 50 mg/L, the adsorption capacity of Ag@Wool-AO can reach 92.49 mg/g. The adsorption process followed the pseudo-second-order kinetic model and Langmuir adsorption isotherm model. Using the Langmuir model, we found the adsorption capacity of Ag@Wool-AO for U-(VI) ions to be 172.71 mg/g. Under simulated seawater conditions, the removal rate of the U-(VI) ion by Ag@Wool-AO is 33.30%. Furthermore, the loaded Ag nanoparticles imparted good antibiofouling properties to the adsorbent by providing hot electrons for the reduction of U-(VI) under the action of photoactivity. The cooperation between the injected hot electrons and the U-(VI) binding site directly promotes the remarkable U-(VI) enrichment of Ag@Wool-AO. In short, the strategy described in this paper provides a green, sustainable, and low-carbon preparation route for the preparation of amidoxime-based adsorbents via the thiol-ene click reaction.