Random Al2O3 nanoparticle-based polymer composite films are investigated as external scattering layers to enhance light extraction from flexible organic light-emitting diodes (OLEDs). We found that the size and concentration of the nanoparticles (NPs) in the polymer film play a crucial role in improving light extraction. It turned out that their increase has a favorable impact on the light output of the devices, as the high concentration of the NPs leads to the formation of large nanoparticle clusters, which, in turn, yield pore-containing films. As a result, light extraction efficiency of the flexible OLEDs on PEN substrates was enhanced by a factor of 1.65 by the incorporation of the scattering layer, with the highest Al2O3 NP concentration of 99 wt%. This outcome is attributed to the reduction of the waveguide mode and total internal reflection at the substrate/air interface induced by the randomly distributed NPs in the flexible scattering layer. Our work demonstrates an efficient, solution-processable, and low-cost light-outcoupling structure for large-area and flexible OLED applications.