Organic arsenic compounds in the environment are a global threat to human health. This threat has created the urgency to develop highly efficient adsorbents with both high adsorption capacity and versatile removal of different arsenic compounds. A novel 1D zinc(II) coordination polymer, formulated as Zn2(datrz)2(bpy)Cl2 (BUC‐70) (datrz = guanazole, bpy = 4,4′‐bipyridine), was successfully synthesized through slow evaporation at room temperature. BUC‐70 exhibited an excellent adsorption capacity toward p‐arsanilic acid (p‐ASA) and roxarsone (ROX) in water, which could be ascribed to As–O–Zn bonding interactions and strong hydrogen‐bonding interactions between the organic arsenics and BUC‐70. The maximum adsorption capacities toward p‐ASA and ROX were 738 and 937 mg·g−1, respectively. BUC‐70 was effective in the removal of p‐ASA and ROX at low concentrations (<5 mg·l−1) from the simulated p‐ASA and ROX wastewater. Furthermore, the as‐synthesized BUC‐70 exhibited good adsorption property toward p‐ASA and ROX in wastewater simulated by lake water and tap water. After adsorptive treatment using BUC‐70, the concentrations of both p‐ASA and ROX were lower than the required concentrations of the drinking water standard of the World Health Organization and the surface water standard of China. Continuous‐flow, fixed‐bed column experiments were performed using BUC‐70 loaded on cotton as packing material to explore the potential large‐scale application.