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The on-site monitoring of phosphate is important for environmental management. Conventional phosphate detection methods are not appropriate to on-site monitoring owing to the use of complicated detection procedures, and the consequent high cost and maintenance requirements of the detection apparatus. Here, a highly sensitive fluorescence-based method for phosphate detection with a wide detection range was developed based on a luminescent aluminum-based metal-organic framework (Al-MOF). The Al-MOF was prepared by introducing amine functional groups to conventional MIL to enhance phosphate binding, and exhibited excellent fluorescence properties that originated from the ligand-to-metal charge transfer (LMCT). The detection limit was as low as 3.25 µmol/L (0.10 mg/L) and the detection range was as wide as 3–350 µmol/L (0.10–10.85 mg/L). Moreover, Al-MOF displayed specific recognition toward phosphate over most anions and metal cations, even for a high concentration of the co-existent ions. The mechanism of phosphate detection was analyzed through the characterization of the combination of Al-MOF and phosphate, and the results indicated the high affinity between Al-O and phosphate inhibited that the LMCT process and recovered the intrinsic fluorescence of NH2−H2BDC. The recovery of the developed detection method reached a satisfactory range of 85.1%–111.0%, and the feasibility of on-site phosphate detection was verified using a prototype sensor for tap water and lake water samples. It was demonstrated that the prepared Al-MOF is highly promising for on-site detection of phosphate in an aqueous environment. [ABSTRACT FROM AUTHOR]