Organic light-emitting diodes (OLEDs) containing a transparent ultrathin layer of oxidized silver as a hole-injecting layer, placed between a indium–tin-oxide (ITO) electrode and the hole-transporting layer, were fabricated, and their electrical and luminescent properties were investigated. The OLEDs had a structure that consisted of an ITO layer; followed by an ultrathin Ag layer oxidized by a ultraviolet (UV)–ozone surface treatment; a N,N′-di-[(1-naphthyl)-N,N′-diphenyl]-1,1′-biphenyl)-4,4′-diamine (α-NPD) layer; a 5,6,11,12-tetraphenylnaphthacene (rubrene)-doped 9,10-diphenylanthracene (DPA) layer; a tris-(8-hydroxyquinoline) aluminum (Alq3) layer; a lithium fluoride (LiF) layer; and a Al layer. The operating voltages of the OLEDs with the oxidized Ag (i.e., AgOx) layer were drastically lower than those of the layer-free OLEDs, because the AgOx layer, which had high oxidizability, contributed to hole injection as it oxidized the surface of the α-NPD layer. However, the external quantum efficiency of the OLEDs with the AgOx layer was lower than that of the AgOx layer-free OLEDs, suggesting that the carrier balance (i.e., the balance between the holes and electrons) became uneven in the emission layer, owing to the insertion of the AgOx layer. It was assumed that this imbalance resulted from the number of holes in the emission layer being higher because of the increase in hole injection in the AgOx layer.