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Abstract Iodine is widely used as an antimicrobial reagent for water disinfection in the wilderness and outer space, but residual iodine and iodide need to be removed for health reasons. Currently, it is challenging to remove low concentrations of iodine and iodide in water (≈5 ppm). Furthermore, the remediation of iodine and iodide across a broad temperature range (up to 90 °C) has not previously been investigated. In this work, we report a nitrate dimer‐directed synthesis of a single‐crystalline ionic hydrogen‐bonded crosslinked organic framework (H_COF‐7). H_COF‐7 removes iodine and iodide species in water efficiently through halogen bonding and anion exchange, reducing the total iodine concentration to 0.22 ppm at room temperature. Packed H_COF‐7 columns were employed for iodine/iodide breakthrough experiments between 23 and 90 °C, and large breakthrough volumes were recorded (≥18.3 L g⁻¹). The high iodine/iodide removal benchmarks recorded under practical conditions make H_COF‐7 a promising adsorbent for water treatment.