2-Phenylpyrimidine skeleton-based multifunctional electron-transport materials are designed and synthesized. By using these materials and green phosphorescent emitter, fac-tris(2-phenylpyridine)iridium [Ir(ppy)(3)], extremely efficient green organic light-emitting devices are developed. The devices show the efficiencies of 128 lm W(-1) (105 cd A(-1)) at 100 cd m(-2) and 96 lm W(-1) (99 cd A(-1)) at 1000 cd m(-2).