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Novel D–σ–A molecules were developed as single hosts to achieve high performances in monochrome and white organic light-emitting diodes., Two novel D–σ–A host materials 11,11-bis(9-phenyl-9H-carbazol-3-yl)-11H-benzo[4,5]imidazo[1,2-a]indole (BII–BCz) and 4,4′-(11H-benzo[4,5]imidazo[1,2-a]indole-11,11-diyl)bis(N,N-diphenylaniline) (BII–TPA) are synthesized by using the sp3 carbon attached to a newly designed 11H-benzo[4,5]imidazo[1,2-a]indole building block to link two electron-donating groups. The resulting materials feature high triplet energy levels, good thermal properties and suitable photophysical properties as universal hosts for full-color phosphorescent organic light-emitting diodes (OLEDs). Both BII–BCz and BII–TPA reveal excellent performances in blue, green, yellow, orange and red phosphorescent OLEDs with the same device structure. The employment of the new D–σ–A materials as single hosts in white OLEDs with a simple device structure allows us to achieve state-of-the-art performances. A single-emissive-layer white device based on BII–BCz demonstrates the highest performance with an external quantum efficiency up to 28.2% at 1000 cd m–2. Furthermore, this device displays extremely stable emission spectra, with a ΔCIE of only (0.009, 0.005) from 1000 to 10 000 cd m–2.