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Fe3O4 has been demonstrated to be an efficient p-dopant in improving the performance of organic light-emitting devices. This paper investigates in detail the role of Fe3O4 in improving the hole injection and the hole transport by the ultraviolet/visible/near-infrared absorption, x-ray, and ultraviolet photoelectron spectroscopy. The results demonstrated that Fe3O4 as a p-dopant has different effectiveness when it is doped into different host materials. The improved properties of the OLEDs with the p-doped N, N'-diphenyl-N,N'-bis (1,1'-biphenyl)-4,4'-diamine layer is mainly due to the enhanced hole injection through the lowering of the hole injection barrier, while the enhanced hole transport plays a more important role for the OLEDs with the p-doped 4,4',4”-tris (3-methylphenylphenylamino) triphenylamine due to their higher ability in the formation of charge transfer complex.