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Herein we report a novel design philosophy of tandem OLEDs incorporating a doping-free green phosphorescent bis[2-(2-pyridinyl-N)phenyl-C](acetylacetonato)iridium(III) (Ir(ppy) 2 (acac)) as an ultrathin emissive layer (UEML) into a novel interface-exciplex-forming structure of 1,1-bis[(di-4-tolylamino)phenyl]cyclohexane (TAPC) and 1,3,5-tri(p-pyrid-3-yl-phenyl)benzene (TmPyPB). Particularly, relatively low working voltage and remarkable efficiency are achieved and the designed tandem OLEDs exhibit a peak current efficiency of 135.74 cd/A (EQE = 36.85%) which is two times higher than 66.2 cd/A (EQE = 17.97%) of the device with a single emitter unit. This might be one of the highest efficiencies of OLEDs applying ultrathin emitters without light extraction. Moreover, with the proposed structure, the color gamut of the displays can be effectively increased from 76% to 82% NTSC if the same red and blue emissions as those in the NTSC are applied. A novel form of harmonious fusion among interface exciplex, UEML, and tandem structure is successfully realized, which sheds light on further development of ideal OLED structure with high efficiency, simplified fabrication, low power consumption, low cost, and improved color gamut, simultaneously.