Single‐band ratiometric (SBR) thermometry has recently emerged as a powerful alternative to its dual‐emission counterparts because it can avoid the large uncertainties related to the emission spectral overlap or light absorption/scattering by the medium. Herein, a novel SBR thermometric scheme in Sc2Mo3O12:Eu3+ nanosheet that depends on thermal enhancement of charge‐transfer state absorption between O2− and Eu3+ is reported. Mechanistic investigation reveals the vital role of the lattice negative thermal expansion (NTE) for thermally enhanced Eu3+ emissions according to the configuration coordinate model. In contrast, serious thermal quenching of Eu3+ emissions is detected under the excitation wavelength corresponding to ground state absorption. Such excitation wavelength‐dependent thermal behavior of luminescence enabled SBR thermometry with high sensitivity and resolution (Sr = 2.0% K−1, δT = 0.121 K at 363 K). Finally, the applicability of the proposed SBR model to real‐world sensing scenarios is demonstrated using the as‐fabricated flexible thin‐film, offering accurate and real‐time temperature detection at the local hotspot in the electronic component.
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