Two soluble bipolar host materials (mCP-BPBI and CP-QPBI), comprising different proportions of hole-transporting carbazole and electron-transporting benzimidazole, were synthesized. Their thermal, physical, and electrochemical properties were characterized. The designated bulky star-shaped structures efficiently suppress the direct intramolecular interaction between the donor and acceptor subunits to give high triplet energies. Through computational studies, varying the ratio of hole- and electron-transporting moieties could significantly change the carrier injection/transporting abilities and charge balance properties of the host materials. Indeed, CP-QPBI with more benzimidazole units shows extremely enhanced current density at the same voltage when compared to mCP-BPBI. The operating voltage of solution-processed phosphorescent light-emitting diodes with CP-QPBI as host were dramatically reduced by ∼3 V compared with the similar devices of mCP-BPBI. At the same time, the power efficiencies were improved for 2-2.5 times at the corresponding voltage. Importantly, both blue and green devices maintain their high efficiencies even at brightness up to 1000 cd m(-2), which clearly demonstrates that the new strategy applied to improve electron-transporting ability and charge-balance property of the solution-processable host material by tuning the ratio of donor and acceptor unit is profitable.