Effective sequestration of bromine holds great promise for the chemical industry's safe expansion, environmental preservation, and public health. However, attaining this goal is still challenging due to the serious drawbacks of existing adsorbents such as limited capacity, low retention efficiency, and sluggish uptake kinetics. Herein, we report a strategy-driven systematic study aimed at significantly enhancing multiple host-guest interactions to obtain functionalized covalent-organic frameworks for the efficient sequestration of bromine. Results showed that the presence of specific quantities of selective binding sites of the porous frameworks afford stronger host-guest interactions and therefore higher bromine adsorption capacities. The developed framework exhibits high bromine sorption capacity of up to 5.16 g g-1 in the vapor phase and 8.79 g g-1 in the aqueous phase under static adsorption conditions with fast kinetics, large distribution coefficient (Kd ∼105 mL g-1), high retention efficiency and reusability. Moreover, the adsorbent is able to sequestrate trace bromine (from 13 ppm to below 4 ppm) from aqueous medium with fast adsorption kinetics (86.3% within less than 3 h) and demonstrates the selective extraction of bromine over iodine under both static and dynamic conditions. These results were further utilized to demonstrate recycling-selective and highly efficient bromine capture from a real-water system, exhibiting excellent scalability and affordability, as exemplified using COF membranes in a continuous flow-through process.