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High salinity has plagued wastewater treatment for a long time by hindering pollutant removal, thereby becoming a global challenge for water pollution control that is difficult to overcome even with massive energy consumption. Herein, we propose a novel process for rapid salinity-mediated water self-purification in a dual-reaction-centers (DRC) system with cation-p structures. In this process, local hydrogen bond networks of H2O molecules can be distorted through the mediation of salinity, thereby opening the channels for the preferential contact of pollutants on the DRC interface. As the result, the elimination rate of pollutants increased approximately 32-fold at high salinity (100 mM) without any external energy consumption. Our findings provide a novel technology for high-efficiency and low-consumption water self-purification, which is of great significance in environmental remediation and even fine chemical industry. [ABSTRACT FROM AUTHOR]