With the aim to design and synthesize cyclometalated Ir(III) complexes with near-infrared (NIR) emission, a series of ppy-type ligands with fluoranthene unit have been synthesized bearing different aromatic nitrogen heterocycles of isoquinoline, quinoline, pyridine and benzo [d]thiazole. With these organic ligands, four [Ir (ppy)2 (acac)] complexes are prepared named as IrFTIQ, IrFTQL, IrFTPY and IrFTBZ. In solution, IrFTIQ can emit NIR phosphorescence at 738 nm, while IrFTQL (ca. 692 nm), IrFTPY (ca. 670 nm) and IrFTBZ (ca. 690 nm) are typical deep-red emitters. It should be noted that all these fluoranthene-based cyclometalated Ir(III) complexes show good electrochemical stability indicated by their reversible redox procedures. When doped in the emission layer of OLEDs, IrFTIQ and IrFTBZ can furnish NIR electroluminescence (EL) at 748 nm and 700 nm, respectively, while the devices with IrFTPY as emitter can furnish deep-red EL. Critically, the optimized OLED doped with IrFTIQ can achieve maximum external quantum efficiency (EQE) as high as 5.01 % and a radiance up to 6284 mW Sr−1 m−2. Critically, the NIR OLEDs based on IrFTIQ can furnish EL with NIR component (NIR%) of a total spectrum > 99 %. All these encouraging results definitely demonstrate the effectiveness of our molecular design strategy for the new-type Ir(III) NIR phosphorescent complexes and the great potential of the fluoranthene group in developing high-performance Ir-based NIR phosphors for OLEDs.