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Breaking hydrogen bond in metal free carbon nitride (CN) to increase peroxymonosulfate (PMS) adsorption for surface-mediated electron transfer has been challenging. Herein, we incorporated N−C N monomer into CN to break hydrogen bond by the introduction of polyvinylpyrrolidone (PVP). The developed nonradical oxidation system achieved selective decomposition of highly hydrophilic contaminants and efficient removal of chemical oxygen demand (58.0%), total phosphorus (88.1%), ammonia nitrogen (100.0%) and total nitrogen (67.8%) from the secondary effluent in a continuous flow reactor. This was attributed to that the breakage of hydrogen bond accelerated the redistribution of electron densities at C and N sites, leading to an increase in the adsorption energy of N site to PMS. This promoted the formation of PVP/CN-PMS* complex for the selective and efficient removal of organics and inorganics. This work provided a new perspective for the selective and long-term treatment of practical wastewater. [Display omitted] • Surface-mediated electron transfer system was constructed by breaking hydrogen bond. • The effect of hydrogen bond in carbon nitride on PMS activation pathway was revealed. • PVP/CN/PMS/vis system selectively remove highly hydrophilic contaminants. • The efficient and continuous flow treatment of practical wastewater was achieved. [ABSTRACT FROM AUTHOR]