In this report, C60/pentacene was applied as the nondoped charge generation layer (CGL) to achieve excellent performance of TOLEDs with using Al and MoO3 layer as the electron and hole injection layers, respectively. Green phosphorescence TOLEDs with the structure of ITO/NPB/mCP∶Ir(ppy)3/TPBi/Al/C60/pentanece/MoO3/NPB/mCP∶Ir(ppy)3/TPBi/Cs2CO3/Al were fabricated. Experimental results show that inserting Al and MoO3 layer can effectively increase the charge injection capacity of organic CGL, and improve the luminance and current efficiency of TOLEDs. The turnon voltage of TOLEDs is much lower than that of singleunit device, but the current efficiency is more than 2 times as that of the singleunit device. TOLEDs can exhibit excellent photoelectric performance when the thickness of Al/C60/pentanece/MoO3 is 3, 15, 25 or 1nm. The maximum luminance and current efficiency are 7920.0cd/m2 and 16.4cd/A, respectively.