Environmentally friendly, high adsorption efficiency, and recyclable adsorbents meet the actual needs of organic dye wastewater treatment. Driven by noncovalent interactions between chitosan (CS) and 5,10,15,20‐tetra(4‐hydroxyphenyl) porphyrin sodium (THPPNa) under acidic conditions, a supramolecular polymer network is constructed. The supramolecular polymer network is applied as an excellent adsorbent for the removal of organic dyes from water with high efficiency. In addition, the supramolecular adsorbent shows excellent selectivity for the removal of organic anionic dyes from the mixtures of organic anionic and cationic dyes in water. Furthermore, the removal efficiency of anionic dyes of the network adsorbent keeps over 95% even after five adsorption–desorption cycles, indicating its reusability. This supramolecular polymer network shows its great potential as a low‐cost, effective, and selective adsorbent for removing organic dyes from water.