An ultrathin polyethylene nanofibrous membrane (UTPENFM) substrate with a large specific surface area was prepared by biaxial stretching, and the modified UTPENFM adsorbent, called the AO−UTPENFM, was successfully prepared by a two-step grafting method. By adjusting the pore structure of the matrix material by biaxial stretching, the area of functional groups can be exposed to the maximum extent on the membrane surface layer so as to realize the rapid adsorption process of uranium. Herein, in the simulated seawater with a uranium concentration of 8 ppm, the adsorption capacity is 172.88 mg/g for 6 h. Meanwhile, the adsorption capacity of uranium is 3.38 mg/g in natural seawater for 7 days, which indicates that the adsorption of uranium by the UTPENFM-g-PHEA-(PAO-co-PAA) (AO−UTPENFM) adsorption material is an ultrafast adsorption process. The AO−UTPENFM, with its higher specific surface area and larger pore structure, provides abundant space for the entry of uranyl ions, which can accelerate the adsorption rate of uranium, indicating that the AO−UTPENFM is a promising adsorbent for uranium extraction from natural seawater. These findings provide insights into uranium extraction from seawater and bode well for the potential of uranium extraction from seawater using ultrathin polymer-based adsorbents.