Sluggish　charge　kinetics　and　NO　diffusion　largely　restrict　the　photocatalytic　efficiency　of　low-dose　NO　removal　by　layered　carbon　nitride　(CN).　Herein,　a　novel　poly(heptazine　imide)-based　CN　(CN-NaLi)　with　enlarged　interlayer　spacing　was　fabricated　by　an　easy,　efficient　and　unique　molten-salt　approach.　The　charge　flows　induced　by　the　poly(heptazine　imide)　structure　can　be　delocalized/separated/transferred,　resulting　in　a　signif-icantly　boosted　efficiency　of　charge　kinetics.　The　enlarged　interlayers　distance　of　CN-NaLi　reduced　the　charge　-recombination　probability　and　promoted　NO　diffusion/adsorption/activation.　Accordingly,　abundant　separated　light-induced　electrons　can　be　supplied　to　react　and　activate　the　O-2　molecules.　Meanwhile,　large　amounts　of　adsorbed　NO　were　fixed　and　converted　into　the　intermediate　product　during　the　same　time　compared　with　unmodified　CN.　The　reduced　energy　barrier　endowed　CN-NaLi　with　superior　visible-light-driven　performance,　high　stability,　and　decreased　generation　of　toxic　products　in　NO　purification.　This　research　highlighted　the　vital　concerns　in　affecting　the　interlayer　NO　diffusion/adsorption/activation　and　charge　delocalization/separation/　transportation.