The first luminescent two-dimensional MOF nanosheets NTU-9-NS Ti2(HDOBDC)2(H2DOBDC) (H2DOBDC=2,5dihydroxyterephthalic acid) fabricated via top-down delamination have been realized for fast-response and highly sensitive sensing of Fe 3+ . The highly dispersive nature and high accessible active sites on the surface of the 2D NTU-9-NS nanosheets enable them to have close contact with targeted metal ions, which led to fast-response and highly sensitive sensing of Fe 3+ ions, with the response time within seconds and the best detection limit performance of 0.45 µM among MOF materials. The fast-response and highly sensitive Fe 3+ sensing based on the NTU-9-NS nanosheets sensor material highlights the very promise of luminescent sensing applications of two-dimensional MOF nanosheet approach. This work contributes to develop the research on two-dimensional MOF nanosheets materials with targeted and specific recognition for the biological and environmental luminescent sensors.