Abstract: | Color‐tuning for phosphorescent emitters in organic light‐emitting diodes (OLEDs) across the entire visible spectrum is prerequisite to fulfil flexible full‐color displays and white solid‐state lighting. Heteroleptic 2‐phenylpyridine‐type (ppy‐type) Ir(III) and Pt(II) complexes as phosphorescent emitters have been well exploited in the electroluminescence (EL) field due to their outstanding EL performance. Furthermore, the photophysical characters of these heteroleptic Ir(III) and Pt(II) complexes are generally dominated by the nature of cyclometalating ppy‐type ligands. Accordingly, either sophisticated modification or judicious combination of different cyclometalating ppy‐type ligands will provide a wonderful platform to tune their emission color. In this personal account, we put a special emphasis on our contributions to the novel color‐tuning strategies in these heteroleptic ppy‐type Ir(III) and Pt(II) complexes. In addition, afforded by our novel color‐tuning strategies, ambipolar character or enhanced electron injection/transport (EI/ET) features can be furnished to bring high EL performances. |