As a heavy metal ion, excessive aluminum ions pose a serious threat to human health and the ecological environment. Developing a simple, efficient, and fast detection method to detect the content of aluminum ions is of great significance, especially for ensuring human health and ecological safety. Herein, the mixed rare earth metal–organic framework (Ce0.74Eu0.26TPTC and Ce0.62Eu0.38TPTC) were prepared based on simple ligand 1,1′:4′,1″‐Terphenyl‐2′,4,4″,5′‐tetracarboxylic acid (H4TPTC). The Ce0.74Eu0.26TPTC and Ce0.62Eu0.38TPTC have dual luminescence centers, which can be used as ratio fluorescent probes to detect Al3+ ions, making the detection results more accurate and reliable. Therefore, this work can promote the further development of rare earth‐based MOFs in the detection of heavy metal ions.