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Fe3+ is a promising dopant for designing near‐infrared (NIR) phosphors due to its broadband emitting, non‐toxic, and inexpensive properties. However, the 4E (4D) and 4E + 4A1 (4G) levels of Fe3+ ions are independent of the crystal‐field parameter, and the spectral regulation has become a huge challenge. Herein, a broadband NIR‐emitting phosphor Ca2.5Hf2.5(Ga, Al)3O12: Fe3+ is successfully developed toward long‐wave ultraviolet (LWUV) light‐pumped NIR phosphor‐converted LED (pc‐LED). Significantly, the excited transition reverse of Ca2.5Hf2.5Ga3O12: Fe3+ can be realized by simply adjusting Fe3+ concentration, which results in the largely enhanced excitation around 410 nm and matches well with the commercial LWUV LED. Moreover, Ca2.5Hf2.5Ga3O12: Fe3+ can exhibit a broadband NIR emission centered at 770 nm with optimized doping content at 0.01 mol%, which are demonstrated to ascribe to Fe3+ occupying both octahedral Hf 4+ and tetrahedral Ga3+ sites. Further, a simple cation modulation strategy is proposed to successfully break the lattice symmetry around Fe3+ ions and largely enhance the NIR‐emission intensity to 200% as much as before. Finally, a NIR pc‐LED is fabricated by employing Ca2.5Hf2.5Ga3O12: Fe3+, Al3+ coating on a 410 nm LED chip, which shows great potential in non‐destructive inspection applications. [ABSTRACT FROM AUTHOR]