In this work, we performed the investigation on surface modification of indium tin oxide (ITO) anode by depositing MoO3 interface layer and treating with low pressure plasma. Experimental results revealed both low pressure oxygen plasma treatment and MoO3 interface layer are efficient in facilitating the injection of holes, while both modifications increase the ITO surface roughness. Interestingly, the electroluminescent (EL) device with 3nm MoO3 layer displayed the highest EL performances, which were even higher than those of the device with both modifications. By optimizing the selection of gas, treatment time, and applied electric field intensity of low pressure plasma treatment, the combination of 3nm MoO3 layer and 2min low pressure nitrogen plasma treatment at 4000Vm−1 was demonstrated to be most efficient in depressing the unexpected leakage current without sacrificing the injection rate of holes.