An optical scattering layer, consisting of a Si3N4 nano-pillar array and a spin-coated hydrogen silsesquioxane (HSQ) planarization layer, was introduced to an organic light-emitting diode (OLED) substrate to increase the out-coupling efficiency. After plasma enhanced chemical vapor deposition (PECVD) of the Si3N4 layer, the nano-pillar array was created using nanoimprint lithography and reactive ion etching. As the Si3N4 pillar array has a refractive index of 2.0, photons generated in the organic layer are scattered by the Si3N4 structures and thus have a higher chance of being emitted from the device. The spin-coated HSQ planarization layer produces a flat substrate, which is essential for depositing a uniform organic material layer and assuring the electric conductivity of the transparent conducting oxide (TCO) layer. In this study, Si3N4 nano-structures with a height of 100 or 300 nm were used to enhance the out-coupling efficiency of the OLED devices. Although the electrical conductivity of the TCO layer deposited on the light scattering layer was slightly degraded, the OLED devices formed with the light scattering layer exhibited a higher luminous power at given electrical power. Consequently, the use of a planarized 300-nm-thick Si3N4 layer increased the external quantum efficiency of the OLED device by 50% at 10,000 cd/m2 compared to the reference OLED device fabricated on a flat glass substrate.