Polymer light-emitting diodes (PLEDs) having indium tin oxide (ITO)/PEDOT:PSS [poly(3,4-ethylenedioxythiophene)-polystyrene sulfonate]/PVK [poly-vinylcarbazole]:PFO-poss [poly(9,9-dioctylfluorene) end capped by polyhedral oligomeric silsesquioxane]/TPBI [2,2',2”-(1,3,5-benzinetriyl)-tris(1-phenyl-1-H-benzimidazole)]/LiF/Al structures were prepared on plasma-treated ITO/glass substrates using spin-coating and thermal evaporation methods. The effects of the plasma treatment on the ITO films to the optical and electrical properties of the PLEDs were examined. The sheet resistance of the ITO films decreased with an increasing radio frequency (RF) plasma intensity from 20 to 200 W under a 20 mTorr Ar + O2 gas (50:50 vol.%) pressure. The work function of the ITO films without plasma treatment was 4.97 eV, and increased to about 5.16–5.23 eV after the plasma treatment of the films. The surface roughness improved with increasing plasma intensities. The luminance and current efficiency of the PLEDs were improved when the devices were prepared on the plasma-treated ITO/glass substrates. The maximum current density and luminance for the PLEDs was obtained at a 150-W RF plasma intensity; they were 310 mA cm−2 and 2535 cd m−2 at 9 V, respectively. The Commission Internationale d'Eclairage (CIE) color coordinates were found to be x, y = 0.17, 0.06–0.07, showing a good blue color.