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[Display omitted] • Magnetic-single-molecular material is used for uranium adsorption for the first time. • Fully exposure of functional group guarantees high uranium adsorption capacity. • The magnetism of the adsorbent endows it with high recyclability and reusability. • High adsorption capacity of 84.31 mg/g is achieved in simulated nuclear wastewater. • Highest uranium adsorption speed is achieved in simulated nuclear wastewater. Highly efficient treatment of uranium contamination is of great importance for the sustainable development of the environment. The recovery of uranium by adsorbents is a feasible strategy for treating uranium contamination. However, due to insufficient exposure of the contact interfaces, currently available adsorbents usually take extremely long time for uranium adsorption. Herein, a magnetic-single-molecular amidoxime adsorbent M−AO−Fc is fabricated for highly efficient recovery of uranium from nuclear wastewater by endowing the amidoximated cyanoferrocene with magnetism. The adsorbent M−AO−Fc shows a maximum uranium adsorption capacity of 510.60 mg/g in uranium solution. In an acidic simulated nuclear wastewater containing a large number of interfering ions, M−AO−Fc also shows a high uranium adsorption capacity of 84.31 mg/g within a short equilibrium time of 60 min. The full dispersion of M−AO−Fc and full exposure of functional groups are the critical reasons for the excellent uranium adsorption performance. Attributing to the magnetism of M−AO−Fc, this adsorbent can be efficiently recovered by magnetic recovery and shows high reusability. This study proves that the magnetic-single-molecule would be a promising adsorbent for uranium recovery and opens up a new direction for designing a uranium adsorbent. [ABSTRACT FROM AUTHOR]