ABSTRACT Temperature in various scientific and industrial applications requires accurate detection and measurement. Herein, a range of novel isostructural lanthanide‐based metal–organic frameworks (Ln‐MOFs), [Eu x Tb 2−x (3,5‐pdc) 3 (phen) 2 (H 2 O) 2 ] n (x = 0, Tb‐MOF ; x = 2, Eu‐MOF ; x = 0.002, 0.010, 0.020, 0.040, 0.080, Eu x Tb 2−x ‐MOF ), were solvothermally synthesized using 3,5‐pyridinedicarboxylic acid (3,5‐H 2 pdc) and 1,10‐phenanthroline (phen) as ligands. Based on binuclear second building units, Ln‐MOFs exhibited 2D layered structure with sql topology. The luminescent properties of series Ln‐MOFs show systematic tuning shifted from green to red by adjusting the ratio of Eu 3+ to Tb 3+ . The temperature sensing experiments showed that Eu 0.020 Tb 1.980 ‐MOF exhibited self‐calibration temperature response in a range of 293–413 K, achieving maximum relative sensitivity ( S r ) 2.46%·K −1 at 413 K, outscoring many state‐of‐the‐art temperature sensors reported in literature. This study poses great promise of the newly designed Eu 0.020 Tb 1.980 ‐MOF for the ultra‐sensitive temperature sensing in diverse and large‐scale applications.

Self‐Calibration Temperature Sensing and Color Tunable Emission in a Bimetallic Lanthanide Metal–Organic Framework