Two novel ionic red/near-infrared Ir(III) complexes (Ir1 and Ir2) were reasonably designed and prepared using 2-(1-isoquinolinyl)-9,10-anthraquinone as the main ligand and 4,4′-dimethyl-2,2′-bipyridyl and 4,4′-dimethoxy-2,2′-bipyridyl as the auxiliary ligands, respectively. Both complexes showed bright phosphorescence in solution (peak at 618 nm with a shoulder at 670 nm). Interestingly, the phosphorescence peak of two Ir(III) complexes showed a blue-shift of about 36 nm after being ground. Simultaneously, both complexes exhibited mechanical force-induced enhanced emission, and the intensity of the luminescence for Ir1 and Ir2 increased by around two times compared to the one before being ground, respectively. Powder X-ray diffraction (PXRD) and time-dependent density functional theory (TD-DFT) calculation were utilized to understand well the mechanism of this phenomenon and suggested that the destruction of the well-ordered crystalline nature and the decline in triplet-triplet annihilation maybe responsible for the pressure-induced blue-shift and the enhancement of the phosphorescence.