Broadband near-infrared (NIR) phosphors are crucial components of NIR phosphor-converted light-emitting diode (pc-LED) sources for various smart spectroscopy applications. However, developing an efficient, tunable, and inexpensive broadband NIR phosphor with sufficient spectral coverage remains a great challenge. In this work, a cubic phosphate K2AlTi(PO4)3 with highly structural rigidity was chosen as host material for Cr3+ substitution to create an efficient NIR emission. Synthesizing this compound, the obtained material exhibits a broadband NIR emission covering 700-1200 nm with a peak wavelength ranging from 820 to 860 nm depending on the Cr3+ substituting concentration. The Cr3+ concentration optimized sample possesses a photoluminescence quantum yield (PLQY) of 76.4% with an emission peak centered at 857 nm and a full width at half-maximum (fwhm) of 184 nm under 464 nm exaction, demonstrating an efficient and relatively long-wavelength NIR emission with wide spectral coverage. This broadband NIR emission is mainly derived from a single kind of emission center deduced from spectral analysis, luminescence dynamics, and first-principle calculations. Using this material, the fabricated NIR pc-LED device presents an excellent NIR output power and NIR photoelectric conversion efficiency, making this material attractive in practical applications of night-vision and bioimaging. Therefore, this work not only provides a broadband NIR material with superiorities of low cost, high efficiency, wide-range tunability, wide spectral coverage, and relatively long-wavelength NIR emission for spectroscopy applications but also highlights some clues to discover this kind of materials.