Near-infrared (NIR) spectroscopy technology has demonstrated unparalleled efficacy in night vision, iris authentication, plant illumination, food inspection, and various other domains. Nonetheless, the quest for novel phosphors exhibiting superior luminescent efficiency and enduring thermal stability persists as a formidable obstacle. In this study, phosphors MgGaBO4: Cr3+, Al3+ were successfully synthesized by high-temperature solid-phase reaction method. Firstly, starting from MgGaBO4: Cr3+, the crystal field environment around Cr3+ ions was modulated by replacing Ga3+ with Al3+ to further improve the luminescence performance of the phosphor. The emission peak wavelength of MgGaBO4: 0.0075Cr3+,0.005Al3+ phosphor was about 756 nm, the full width at half-maximum (FWHM) was about 174 nm under the blue light excitation of 440 nm. In addition, the luminescence intensity at 100 °C remains at 77.41% of that at room temperature. Finally, the excellent moisture resistance of this phosphor was demonstrated. This work not only introduces a novel broadband NIR phosphor with promising application potential in advanced agricultural lighting but also proposes a synergistic enhancement strategy for effectively improving the performance of broadband NIR phosphor-converted LED light sources.