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.