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99Tc primarily exists high mobility in the natural aqueous environment due to its extremely high solubility and non-complexing features, which can easily cause radioactive pollution. We herein report a general strategy for constructing a novel resin (SiPAN-PEI) with multiple positive charges nitrogen, exhibiting ultrafast adsorption kinetics (< 3 min), superior adsorption capacities (463.96 mg g−1), and excellent selectivity in the presence of excess competitive anions, which exceed those of most commercial resins. Moreover, based on impressive structure stability in extreme conditions, SiPAN-PEI can still maintain superior adsorption abilities after suffering irradiation, calcination, and immersion in strong acid. In addition, the separation performance kept excellently after five loading-washing-eluting cycles and the total adsorption ratio can still reach 97 %. Outstandingly, SiPAN-PEI can remove most of ReO 4 - from simulated nuclear wastewater through a sequential injection automatic separation system and can reduce the concentration of ReO 4 - to the maximum concentration standard set by the World Health Organization (WHO) in a short time. Leveraging density functional theory calculations and other characteristics clearly elucidated adsorption mechanism of anion-exchange between Cl- and TcO 4 -/ReO 4 -. In terms of superior adsorption property, SiPAN-PEI is demonstrated to be a pretty candidate for 99Tc elimination from wastewater. [Display omitted] • A novel resin SiPAN-PEI was successfully synthesized for selective capture of 99Tc. • SiPAN-PEI exhibited excellent adsorption ability of 99Tc in harsh conditions. • Multiple positive charge nitrogen plays a critical role in capture of 99Tc. • SiPAN-PEI demonstrated efficiency capture of 99Tc in simulated wastewater. [ABSTRACT FROM AUTHOR]