In this work, composite layers comprising two-dimensional MoS2 and graphene oxide (GO) were employed as hole injection layers (HILs) in organic light-emitting diodes (OLEDs). MoS2 was fabricated by the butyllithium (BuLi) intercalation method, while GO was synthesized by a modified Hummers method. The X-ray diffraction patterns showed that the intensity of the MoS2 (002) peak at 14.15A degrees decreased with increase in GO content; the GO (001) peak was observed at 10.07A degrees. In the C 1s synchrotron radiation photoemission spectra, the contributions of the C-O, C=O, and O-C=O components increased with increase in GO content. These results indicated that GO was well mixed with MoS2. The lateral size of MoS2 spanned from a few hundreds of nanometers to 1 mu m, while the size of GO was between 400 nm and a few micrometers. Thus, the coverage of the MoS2-GO composite on the ITO surface improved as the GO content increased, owing to the large particle size of GO. Notably, GO with large size could fully cover the indium tin oxide film surface, thus, lowering the roughness. The highest maximum power efficiency (PEmax) was exhibited by the OLED with MoS2-GO 6:4 composite HIL, indicating that similar contents of MoS2 and GO in MoS2-GO composites provide the best results. The OLED with GO HIL showed very high PEmax (4.94 lm W-1) because of very high surface coverage and high work function of GO. These results indicate that the MoS2-GO composites can be used to fabricate HILs in OLEDs.