A series of solution-processible 2,2′-dimethyl-biphenyl cored dendrimers, namely G1MP, G2MP, and G3MP, is designed and synthesized by tuning the generation of periphery carbazole dendron. The resulting dendrimers all show excellent solubility in common organic solvents, and their high-quality thin films can be formed via spin-coating with a root-mean-square roughness in the range of 0.38–0.54 nm. G3MP, which contains the third-generation carbazole dendron, has the greatest potential among those made here as an ideal universal host for multicolored triplet emitters. G3MP exhibits good thermal stability, with a glass transition temperature of 368 °C, a triplet energy as high as 2.85 eV enough to prevent the loss of triplet excitons, and suitable HOMO/LUMO levels of –5.30/–2.11 eV to facilitate both hole and electron injection and transport. When using G3MP as the host, highly efficient deep-blue, blue, green, and red phosphorescent organic light-emitting diodes (PhOLEDs) are successfully demonstrated, revealing a maximum luminous efficiency up to 18.2, 28.2, 54.0, and 12.7 cd A–1 with the corresponding Commission Internationale de L'Eclairage (CIE) coordinates of (0.15, 0.23), (0.15, 0.35), (0.38, 0.59), and (0.64, 0.34), respectively. The state-of-art performance indicates that dendritic hosts have a favorable prospect of applications in solution-processed white PhOLEDs and full-color displays.