New versatile host materials with good solubility in common organic solvents are greatly desired to promote solution-processable thermally activated delayed fluorescence organic light-emitting diodes. This paper describes the design and synthesis of two new host materials, namely 3'-(9H-carbazol-9-yl)[ 1,1'-biphenyl]-3,5-diylbis(diphenylphosphine oxide) (CDPO) and 3',5'-di-(9H-carbazol-9-yl)-[1,1'-biphenyl]- 3,5-diylbis (diphenylphosphine oxide) (mCPDPO), featuring hole-transporting carbazole and electron-transporting diphenylphosphine oxide (DPO) entities. The donor strength was varied to a constant n-type DPO core to tune the functional properties. The detailed studies proved that the resulting two new materials exhibit excellent solubility in common organic solvents, high triplet energy (>2.80eV), high glass transition temperature (up to 133 degrees C), and good bipolar electronic nature. Consequently, both compounds were used as hosts in solution-processable blue and green thermally activated delayed fluorescence (TADF) OLEDs. In particular, the devices using mCPDPO as a host in the emissive layer showed outstanding performance with a maximum current efficiency, power efficiency, and external quantum efficiency of 35.3 cd A(-1), 17.0 lm W-1 and 15.4% in the blue-emitting diode, and 61.5 cd A(-1), 29.7 lm W-1 and 18.8% in the green-emitting diode, respectively. These results corroborated the potential of carbazole-phosphine oxide derivatives as host materials in solution-processable blue and green TADF OLEDs.