For optical temperature sensing materials, the emission and excitation bands are extremely critical to measure the temperature by fluorescence intensity ratio (FIR) technique. Singly Ln‐doped optical temperature sensing materials exhibit very few emission bands, which greatly constraints their practical applications of FIR technique. Here, the fabricated Pr/Er co‐doped (K0.5Na0.5)NbO3 materials exhibited multi‐color (red‐green) and dual‐mode (downshifting/upconversion) luminescence properties. The temperature sensitivity can be effectively tuned by choosing different emission or excitation bands. The optimized optical temperature sensitivity reached up to 0.0094 K−1, much higher than that of most temperature sensing materials. Besides, the samples also showed excellent luminescence modulation properties based on the photochromic reaction. Under sunlight irradiation, the luminescent switching contrast (ΔRt) of the samples reached more than 60%. These results may provide a guiding role in designing and modulating optical temperature sensing properties for multifunctional materials.

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