The　persulfate-based　nonradical　reaction　process　has　gained　increasing　attention　in　removing　organic　contaminants,　and　the　process　dramatically　needs　affordable,　robust,　high-performance　heterogeneous　catalysts.　Herein,　dimethyl　formamide　(DMF)　incorporated　graphitic　carbon　nitride　(DCN)　was　synthesized.　The　molecular　engineering　of　the　heptazine　unit　in　DCN　improves　the　electron　mobility,　strengthens　the　built-in　electric　field,　and　provides　abundant　active　sites,　thus　enabling　DCN　to　efficiently　activate　PMS　for　organic　degradation,　with　100　%　removal　of　BPA　within　12　min.　The　investigation　of　the　reactive　species　and　electrochemical　properties　confirmed　the　direct　electron　transfer　in　the　PMS　activation　for　organic　degradation　over　DCN.　More　importantly,　DCN　can　be　used　as　a　membrane　catalyst　in　a　flowing　catalytic　unit,　enabling　continuous　water　purification　and　catalyst　regeneration.　This　work　provides　novel　guidance　for　metal-free　catalyst　design　and　profound　insights　into　the　persulfate-based　heterogeneous　catalytic　oxidation　process　for　water　decontamination　technology.　©　2023　Elsevier　B.V.