Due to the low efficiency of traditional sewage treatment methods, the effective removal of zwitterionic fluoroquinolone (FQs) antibiotics is of vital significant for environment protection. In this work, a SO3H-anchored covalent organic framework (TpPa-SO3H) was deliberately designed by linking phenolic trialdehyde with triamine through Schiff reaction, then low-content Tb3+ ions were loaded onto covalent organic framework according to wet-chemistry immersion dispersion method which benefitting for efficient FQs antibiotics uptaking. Tb@TpPa-SO3H functionalized with regularly distributed sulfonic acid groups and terbium ions which could provide difunctional binding sites. Tb3+ sites could capture carboxylic acid group of FQs molecules according to the complexes coordination effect and sulfonic acid sites play a significant role in the adsorption of FQs molecules through electrostatic interaction with amine group. Tb@TpPa-SO3H with dual complementary function sites exhibited ultra-fast adsorption kinetics (< 2 min, average over 99% removing rate) and high adsorption capacities of 989, 956, and 998 mg g−1 for Norfloxacin (NOR), ciprofloxacin (CIP), enrofloxacin (ENR), respectively. Furthermore, Tb@TpPa-SO3H showed excellent selectivity for the adsorption of FQs in tanglesome system. This work not only explored synergistic adsorption in ion-functionalized 2D covalent organic framework with dual binding sites, but also delineated a promising strategy for the elimination of organic pollutants in environmental remediation. Display omitted •A difunctional Covalent Organic Framework Hybrid Material was prepared for efficient uptake of fluoroquinolone antibiotics.•Difunctional Tb@TpPa-SO3H exhibits outstanding adsorption capacity and short adsorption equilibrium time for FQs.•Tb@TpPa-SO3H shows excellent selectivity for the adsorption of FQs in tanglesome systems.•Plausible FQs adsorbed mechanisms were coordination with metal and electrostatic interaction.