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Here, this study successfully fabricates few‐layer MoS₂ nanosheets from (NH₄)₂MoS₄ and applies them as the hole transport layer as well as the template for highly polarized organic light‐emitting diodes (OLEDs). The obtained material consists of polycrystalline MoS₂ nanosheets with thicknesses of 2 nm. The MoS₂ nanosheets are patterned by rubbing/ion‐beam treatment. The Raman spectra shows that {poly(9,9‐dioctylfluorene‐alt‐benzothiadiazole), poly[(9,9‐di‐n‐octylfluorenyl‐2,7‐diyl)‐alt‐(benzo[2,1,3]thiadiazol‐4,8‐diyl)]} (F8BT) on patterned MoS₂ exhibits distinctive polarization behavior. It is discovered that patterned MoS₂ not only improves the device efficiency but also changes the polarization behavior of the devices owing to the alignment of F8BT. This work demonstrates a highly efficient polarized OLED with a polarization ratio of 62.5:1 in the emission spectrum (166.7:1 at the peak intensity of 540 …