Currently,　most　gas　sensors　of　two-dimensional　(2D)　layered　transition　metal　dichalcogenides　(TMDs)　are　only　focused　on　the　surface　adsorption　while　ignoring　their　large　interlayer　active　regions.　The　recovery　time　of　2D　TMDs　gas　sensors　are　relatively　long　due　to　the　limited　interlayer　spacing.　Herein,　the　interlayer-expanded　VS2　(VS2-E,　10　Å)　based　NO2　gas　sensor　with　rapid　response/recovery　(∼15　s)　is　reported　innovatively.　The　response　and　recovery　time　is　1/23　and　1/41　of　the　normal　interlayer　spacing　VS2　(VS2-N,　5.8　Å)　counterparts,　respectively.　VS2-E　with　coexistence　of　T　and　H　phases　shows　the　p-type　semiconductor　features.　In　addition,　the　response　value　of　VS2-E　sensor　is　∼2　to　50　ppm　NO2　at　120　°C,　approximately　twice　that　of　VS2-N.　The　enlarged　interlayer　spacing　of　VS2-E　promotes　the　adsorption/desorption　of　more　NO2　molecules　between　the　interlayers,　leading　to　a　larger　response　and　quicker　response/recovery　for　VS2-E　compared　with　VS2-N.　This　is　also　confirmed　by　a　weaker　binding　energy　(−0.17　eV)　of　NO2　in　VS2-E　layers　than　that　of　VS2-N　(−0.62　eV)　calculated　by　theoretical　calculation.　This　work　enriches　the　interlayer　sensing　mechanism　and　provides　a　significant　guidance　for　the　applications　of　interlayer　regulation　engineering　in　other　2D　layered　gas-sensing　materials.　©　2022　Elsevier　B.V.