Acute toxicity from thallium (Tl) contamination poses significant risks to ecosystems and human health.Purifying Tl(I)-containing smelting wastewater is challenging due to the high mobility of Tl(I) and the complexity of such wastewater.As a soft acid, Tl(I) preferentially interacts with soft bases based on soft-hard interaction principles.In this study, we developed a pyrrolic-nitrogen-carbon sponge (NCS) as a model adsorbent for rapidly removing Tl(I) from complex aqueous environments, leveraging pyrrolic-N as a distinct soft base.The three-dimensional porous architecture of NCS facilitates quick diffusion of Tl(I) to adsorption sites.The optimized NCS-600 adsorbent can purify Tl(I)-contaminated water to drinking standards (< 0.1 μg/L) in just 10 min (at 0.4 g/L, CTl(I) = 100 μg/L), reaching a high adsorption capacity of 252.14 mg/g.Mechanistic anal. showed that pyrrolic-N primarily facilitated Tl(I) adsorption, while the - OH group played a secondary role due to its minor steric hindrance effect.Outstanding performance was observed across wide pH (4-13) and temperature (15-35 °C) ranges, with negligible impacts of competing ions or coexisting organic compoundsNCS-600 reduced 60.806 μg/L of Tl(I) in zinc smelting wastewater to 0.069 μg/L within 30 min and completely removed 8.3 μg/L from natural water in only 3 min.It stably performed over at least 25 cycles.In fixed-bed operation, only 1.5 g of NCS-600 could purify and exceptionally large 10,109-bed volume (262 L) of contaminated water.This study provides a practical method for thorough decontamination of Tl(I)-containing smelting wastewater and offers new insights into designing advanced adsorbents for removing various heavy metals.