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Ho3 /Yb3 : BaMoO4 phosphors with different concentrations were fabricated by a gel combustion method. The upconversion (UC) luminescence, intrinsic optical bistability, and the corresponding mechanisms were reported for the present system. The optical thermometric properties based on red (5F5→5I8) and green (5F4/5S2→5I8) emissions were studied. The sensing sensitivities could be tuned by manipulating the cooperative energy transfer process. The highest absolute sensitivity was 99 × 10 4 K 1 at 573 K, which is larger than that of many previous UC materials.