With　the　development　of　near-eye　displays,　the　demands　for　display　resolution　and　performance　are　increasing.　Quantum　dot　performance　is　virtually　independent　of　pixel　size,　making　it　an　efficient　way　to　display　ultrahigh　resolution.　However,　the　low　efficiency　of　high-resolution　quantum　dot　devices　has　been　an　urgent　technical　bottleneck　to　be　solved.　Here,　we　constructed　a　dense　single-molecule　modification　layer　and　a　leakage　current　blocking　layer　for　high-resolution　devices　using　self-assembly,　thereby　realizing　ultrahigh-resolution,　high-efficiency,　and　stable　high-resolution　quantum　dot　light-emitting　diodes　(QLEDs).　The　peak　external　quantum　efficiencies　of　the　red　devices　are　24.68%　(8759　PPI)　and　19.54%　(26075　PPI),　respectively,　with　an　exceptional　long　lifetime　(T95@1000　nit)　up　to　4871　h.　In　addition,　we　explored　the　feasibility　of　this　modification　strategy　on　non-Cd-based　quantum　dots.　In　conclusion,　our　strategy　effectively　improves　the　performance　of　high-resolution　devices　and　provides　a　superior　approach　for　realizing　near-eye　display　applications.　©　2024　American　Chemical　Society.