Although　two-dimensional　(2D)　transition-metal　dichalcogenides　(TMDs)　exhibit　attractive　prospects　for　gas-sensing　applications,　the　rapid　and　precise　sensing　of　TMDs　at　low　loss　remains　challenging.　Herein,　a　NO2　sensor　based　on　an　expanded　VS2　(VS2-E)/carbon　nanofibers　(CNFs)　composite　(abbreviated　as　VS2-E-C)　with　ultrafast　response/recovery　at　a　low-loss　state　is　reported.　In　particular,　the　impact　of　the　CNF　content　on　the　NO2-sensing　performance　of　VS2-E-C　was　thoroughly　explored.　Expanded　VS2　nanosheets　were　grafted　onto　the　surface　of　hollow　CNFs,　and　the　combination　boosted　the　charge　transport,　exposing　abundant　active　edges　of　VS2,　which　enhanced　the　adsorption　of　NO2　efficiently.　The　activity　of　the　VS2　edge　is　further　confirmed　by　stronger　NO2　adsorption　with　a　more　negative　adsorption　energy　(−3.42　eV)　and　greater　than　the　basal　VS2　surface　(−1.26　eV).　Moreover,　the　exposure　of　rich　edges　induced　the　emergence　of　the　expanded　interlayers,　which　promoted　the　adsorption/desorption　of　NO2　and　the　interaction　of　gas　molecules　within　VS2-E-C.　The　synergism　of　edge　effect　and　interlayer　engineering　confers　the　VS2-E-C3　sensor　with　ultrafast　response/recovery　speed　(9/10　s)　at　60　°C,　high　sensitivity　(∼2.50　to　15　ppm　NO2),　good　selectivity/stability,　and　a　low　detection　limit　of　23　ppb.　The　excellent　“4S”　functions　indicate　the　promising　prospect　of　the　VS2-E-C3　sensor　for　fast　and　precise　NO2　detection　at　low-loss　condition.　©　2023　American　Chemical　Society.