Near‐infrared (NIR) phosphors converted light‐emitting diodes (NIR pc‐LEDs) are ideal NIR sources for versatile applications, which imply the practical significance in tailoring the emission of the NIR phosphors to enhance the performance for specific application. Herein, a paradigm of tailoring the emissions in a series of Cr³⁺‐doped phosphors to match the applications in NIR lighting, detection, and short‐wave infrared sources through combinatorial management of crystal‐field and energy transfer is presented. The emission band largely increases from 84 to 190 nm when the introduction of [MgO6]‐[GeO4] into Y₃Ga₅O₁₂:0.08Cr³⁺ forms Y₃Mg_xGa_5‐2_xGe_xO₁₂:0.08Cr³⁺ through the substitution of [GaO6]‐[GaO4]. Such a large increase in width makes it suitable for near‐infrared lighting to near‐infrared detection. Moreover, the Yb³⁺, Nd³⁺ and Er³⁺ are doped to construct energy transfer with Cr³⁺, broadening the emission infrared region and enhanced thermal stability. An optimized Yb³⁺ emission dominates Y₃Ga₅O₁₂:0.4Cr³⁺,Yb³⁺ phosphor has excellent thermal stability (129%@423 K) and is suitable for high‐power short‐wave infrared sources. The presented work not only provides a series of well‐performed NIR phosphors, but only lights up the avenue for designing the Cr³⁺ emission for specific application.

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