The extraction of uranium from seawater via membrane adsorption is a promising strategy for ensuring a long-term supply of uranium and the sustainability of nuclear energy. However, this approach has been hindered by the longstanding challenge of identifying sustainable membrane materials. In response, we propose a prototypal hybridization strategy to design a novel series of conjugated microporous polymer (CMPO)@collagen fiber membrane (COLM), as decorated with multiple functional groups through an amination. These sustainable and low-cost membrane materials allow a rapid and high-affinity kinetic to capture 90% of the uranium in just 30 min from 50 ppm with a high selectivity of
Kd > 10
5 mL·g
-1. They also afford a robustly reusable adsorption capacity as high as 345 mg·g
-1 that could harvest 1.61 mg·g
-1 of uranium in a short 7-day real marine engineering in Fujian Province, even though suffered from very low uranium concentration of 3.29 µg·L
-1 and tough influence of salts such as 10.77 g·L
-1 of Na
+, 1.75 µg·L
-1of VO
3-etc in the rough seas. The structural evidence from both experimental and theoretical studies confirmed the formation of favorable chelating motifs from the amino group on CMPN, and the intensification by the synergistic effect from the size-sieving action of CMPN and the capillary inflow effect of COLM.