Applications of trivalent rare earth (RE3+)‐doped light sources in solid‐state laser technology, optical communications, biolabeling, and solar energy management have stimulated a growing demand for broadband emission with flexible tunability and high efficiency. Codoping is a conventional strategy for manipulating the photoluminescence of active RE3+ ions. However, energy transfer between sensitizers and activators usually induces nonradiative migration depletion that brings detrimental luminescent quenching. Here, a transparent framework is employed to assemble ordered RE3+‐doped emitters to extend the emission spectral range by extracting photons from a variety of RE3+ ions with sequential energy gradient. To block migration‐mediated depletion between different RE3+ ions, a nanoscopic heterogeneous architecture is constructed to spatially confine the RE3+ clusters via a “nanocrystals‐in‐glass composite” (NGC) structure. This bottom‐up strategy endows the obtained RE3+‐doped NGC with high emission intensity (nearly one order of magnitude enhancement) and broadband near‐infrared emission from 1300 to 1600 nm, which covers nearly the whole low‐loss optical communication window. Most crucially, NGC is a versatile approach to design tunable broadband emission for the potential applications in high‐performance photonic devices, which also provides new opportunities for engineering multifunctional materials by integration and manipulation of diverse functional building units in a nanoscopic region.

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A multi-mode optical thermometer was developed using novel nanocomposite glass ceramics, containing bi-functional NaYF4:Yb3+/Nd3+ and NaAlSiO4:Cr3+ nanocrystals.

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To improve the utilization efficiency of chlorophyll to sunlight, Tm3+/Cr3+ codoped dual‐phase glass‐ceramics are successfully fabricated as a dual‐light conversion material by the conventional melt‐quenching technique with subsequent heat treatment. Exploiting the radius difference in atomic size, Tm3+ and Cr3+ ions have been rationally designed entering into the NaYF4 and NaAlSiO4 crystal phase, respectively, to avoid detrimental energy quenching. The resulted dual‐phase glass‐ceramics exhibit a great emission enhancement compared to the precursor glass. No obvious lifetime degradation in the codoped glass‐ceramic further proves the successful incorporation of Tm3+ and Cr3+ in distinguished crystalline phases. Utilizing the dual‐phase glass‐ceramics, the useless sunlight can be converted into the desired red/blue region and reabsorbed by the chlorophyll. The Tm3+ ions convert ultraviolet light into the blue region, and the Cr3+ ions transfer green light to the red emission. With the utilization of Tm3+/Cr3+ codoped dual‐phase glass‐ceramics in the greenhouse, the photosynthesis process can be promoted, and furthermore, the production of crops can be improved, indicating the potential applications in the field of green agriculture.