In　recent　years,　much　attention　has　been　focused　on　two-dimensional　(2D)　material-based　synaptic　transistor　devices　because　of　their　inherent　advantages　of　low　dimension,　simultaneous　read−write　operation　and　high　efficiency.　However,　process　compatibility　and　repeatability　of　these　materials　are　still　a　big　challenge,　as　well　as　other　issues　such　as　complex　transfer　process　and　material　selectivity.　In　this　work,　synaptic　transistors　with　an　ultrathin　organic　semiconductor　layer　(down　to　7　nm)　were　obtained　by　the　simple　dip-coating　process,　which　exhibited　a　high　current　switch　ratio　up　to　106,　well　off　state　as　low　as　nearly　10−12　A,　and　low　operation　voltage　of　−3　V.　Moreover,　various　synaptic　behaviors　were　successfully　simulated　including　excitatory　postsynaptic　current,　paired　pulse　facilitation,　long-term　potentiation,　and　long-term　depression.　More　importantly,　under　ultrathin　conditions,　excellent　memory　preservation,　and　linearity　of　weight　update　were　obtained　because　of　the　enhanced　effect　of　defects　and　improved　controllability　of　the　gate　voltage　on　the　ultrathin　active　layer,　which　led　to　a　pattern　recognition　rate　up　to　85%.　This　is　the　first　work　to　demonstrate　that　the　pattern　recognition　rate,　a　crucial　parameter　for　neuromorphic　computing　can　be　significantly　improved　by　reducing　the　thickness　of　the　channel　layer.　Hence,　these　results　not　only　reveal　a　simple　and　effective　way　to　improve　plasticity　and　memory　retention　of　the　artificial　synapse　via　thickness　modulation　but　also　expand　the　material　selection　for　the　2D　artificial　synaptic　devices.　©　2021　American　Chemical　Society.