1 of 5) 1600675 emitter combined with sophisticated device engineering, including an appropriate choice of neighboring materials, is absolutely imperative to achieve high η p OLEDs realizing both high η ext and low drive voltages at high brightness over 1000 cd m −2 . While we developed novel pyrimidine conjugated emitters and the devices, Yang's group reported a pyrimidinebased green TADF emitters realizing a high η ext,max close to 25% and an η p of 74 lm W −1 . [16] However, we note that this device showed a high drive voltage of 3.4 V at 1 cd m −2 and a large efficiency roll-off with η p,1000 of 37 lm W −1 at a high brightness of 1000 cd m −2 .Herein, we investigated the structure-property relationships among pyrimidine conjugate emitters revealing an effective molecular design for high-performance OLEDs. Consequently, we successfully developed a highly luminescent pyrimidine conjugate emitter named PXZ-PPM exhibiting a high η ext of over 25%, with low driving voltages at Commission Internationale de l'Eclairage chromaticity coordinates (CIE) of (0.36, 0.58), and exceptionally low efficiency roll-off realizing η ext of over 22% at a high brightness of 1000 cd m −2 . These OLEDs also exhibited an η p of over 110 lm W −1 (84.9 cd A −1 , η ext = 25.1%) while maintaining extremely low voltages of 2.2 V at 1 cd m −2 and 3.0 V at 1000 cd m −2 , and an η p,1000 of 78.3 lm W -1 (75.5 cd A -1 , η ext = 22.3%). These performances clearly exceed those of previous TADF devices and are comparable to those of their stateof-the-art phosphorescent counterparts. [17][18][19][20][21][22][23] So far, our TADF molecules, denoted as Ac-RPM (R = H, CH 3 , and phenyl), were synthesized introducing two 9,10-dihydro-9,9-dimethyl-10-phenylacridine moieties at the 4-and 6-positions with regard to the pyrimidine unit and exhibited high photoluminescent quantum yields (η PL s) of approximately 80% and strong TADF properties. However, all Ac-RPM derivatives showed similar emission peaks (λ em ) around 490 nm and ΔE ST of 0.19 eV. Thus, the structure-property relationships should be clearly identified for effective molecular design and superior OLED performances based on pyrimidine conjugate emitters. With this aim, we designed two novel pyrimidinebased emitters named PXZ-PPM and Ac-NPM (Figure 1). Ac-NPM possessed a piperidine moiety at the 2-position of pyrimidine. In this sense, stronger electron-donating properties are expected to increase the lowest unoccupied molecular orbital (LUMO) levels, thereby leading to wider energy gaps (E g ) as compared to the phenyl-based Ac-PPM emitter. On the other hand, PXZ-PPM possessed phenoxazine (PXZ) moieties