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Efficient capture of uranium(VI) (U(VI)) from seawater is of great significance to the sustainable development of nuclear energy and environmental protection, which is also a serious challenge at present. In this study, hollow Zn/Co zeolitic imidazolate framework (H-ZIF) was decorated on polyacrylamide/sodium alginate (PAM/SA) hydrogel by chelating and covalently crosslinking, and a new type of PAM/SA/H-ZIF hydrogel was synthesized. The combination of PAM/SA and H-ZIF gives PAM/SA/H-ZIF hydrogel excellent mechanical properties, good stability, and abundant surface functional groups, which is beneficial to improving the adsorption properties. The extraction amount of U(VI) by PAM/SA/H-ZIF is 171.14 mg·g−1 at C0 = 99.52 mg·L−1 and pH = 5.0. The adsorption equilibrium is reached in 120 min and the adsorption process fits well with Langmuir isotherm model and pseudo-second-order rate equation. The PAM/SA/H-ZIF also showed good recyclability and stability after 10 cycles of adsorption–desorption. More importantly, the rate of uranium adsorption is 0.196 mg·g−1·day−1 after 30 days, which implies that the PAM/SA/H-ZIF could serve as a potential adsorbent for the development of uranium capture from seawater.
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