Efficient and sustainable methods for 99 TcO 4 − removal from acidic nuclear waste streams, contaminated water, and highly alkaline tank wastes are highly sought after. Herein, we demonstrate that ionic covalent organic polymers (iCOPs) possessing imidazolium-N + nanotraps allow the selective adsorption of 99 TcO 4 − under wide-ranging pH conditions. In particular, we show that the binding affinity of the cationic nanotraps toward 99 TcO 4 − can be modulated by tuning the local environment around the nanotraps through a halogenation strategy, thereby enabling universal pH 99 TcO 4 − removal. A parent iCOP-1 possessing imidazolium-N + nanotraps showed fast kinetics (reaching adsorption equilibrium in 1 min), a high adsorption capacity (up to 1434.1 ± 24.6 mg/g), and exceptional selectivity for 99 TcO 4 − and ReO 4 − (nonradioactive analogue of 99 TcO 4 − ) removal in contaminated water. By introducing F groups near the imidazolium-N + nanotrap sites (iCOP-2), a ReO 4 − removal efficiency over 58% was achieved in 60 min in 3 M HNO 3 solution. Further, introduction of larger Br groups near the imidazolium-N + binding sites (iCOP-3) imparted a pronounced steric effect, resulting in exceptional adsorption performance for 99 TcO 4 − under super alkaline conditions and from lowactivity waste streams at US legacy Hanford nuclear sites. The halogenation strategy reported herein guides the task-specific design of functional adsorbents for 99 TcO 4 − removal and other applications.