In this article, we have demonstrated the hybrid polymer light-emitting diodes (PLEDs) with a sol-gel derived or rf-sputtered ZnO electron transport layer (ETL). For the ZnO films prepared under different conditions, low annealing temperature (300°C) leads to the film amorphous while the polycrystalline films is readily achieved by sputtering. Though the surface roughness can be improved by thermal annealing at 400°C for sputtered films, the release of compressive stress after treatment has shrunk the optical band gap from 3.282 to 3.268 eV. As the ETL in PLEDs, the reduced band gap could increase potential barrier for electron injection and decrease the hole blocking capability. In our cases, luminance larger than 7000 cd/m2 can be obtained in device with pristine sputtered ZnO ETL. It is concluded that crystalline structure of ZnO films is important to facilitate the balance of carrier mobility to obtain high luminance and high efficiency devices.