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[Display omitted] • D201 and IRA-410 resins exhibited fast adsorption kinetics and superior adsorption capacity; • Two resins demonstrated outstanding acid, thermal and irradiation stability; • Two resins could effectively capture ReO4− from simulated Hanford and SRS solutions; • Anion exchange mechanism was elucidated through characterization and DFT calculation. It is still a challenge to capture TcO 4 − from wastewater due to its nature of non-complexing and radioactive. Herein, two types of anion exchange resins (D201 and IRA-410 resin) were selected and explored the adsorption properties for perrhenate (ReO 4 −, as a surrogate for TcO 4 −). It is found that both D201 and IRA-410 resin exhibited fast adsorption kinetic (within 120 min), and superior adsorption capacities, which could reach 671.1 mg g−1 and 561.8 mg g−1 for D201 and IRA-410 resin, respectively. In addition, D201 and IRA-410 resin showed excellent adsorption selectivity for ReO 4 − in the presence of a variety of 1000-fold competing anions (NO 2 −, Cl−, SO 4 2−, and PO 4 3−). Importantly, the two resins still demonstrated outstanding performance after acid/alkaline soaking, calcination procedures as well as high doses of ionizing radiation, they also could remove ReO 4 − from simulated Hanford and SRS wastewater by automatic separation system. Finally, the anion-exchange mechanism was revealed by characterization and DFT. This work demonstrates that D201 and IRA-410 resin are efficient adsorbents for 99Tc removal from nuclear wastewater and provides a basis for designing other novel anion exchange materials for capturing ReO 4 − and TcO 4 −. [ABSTRACT FROM AUTHOR]