In summary, a novel ESIPT-active ɑ-naphtholphthalein-DAMN hydrazone NPDM was successfully developed for enhanced identification specificity and efficiency toward Al 3+ . Molecular tweezers NPDM for Al sensing via ESIPT and CHEF mechanisms, demonstrates merits of dual emissions, splendid selectivity and sensitivity with a very low LOD of 16.3 nM, large Stokes shifts (140 nm/176 nm), and real-time and visualized sensing. The Job's plot, HRMS, 1 H NMR titrations, as well as detailed (TD)DFT calculations elucidated the formation of a 1:2 NPDM-Al 3+ complex with ESIPT "turn-on" process. Intriguingly, NPDM-Al 3+ ensemble can also be utilized as a subsequent fluorescence tweezers for the selective and sensitive recognition of F -anions. Basing on this reversible property, an advanced molecular memory device was fabricated. Moreover, benefiting from the excellent optical performances and biocompatibility, NPDM was efficiently applied in imaging the intracellular Al 3+ and F -ions in Hela cells with good resistance to oxidative stress, especially the OCl -and ONOO -species. More importantly, it is the first reported smart tweezers capable of detecting the Al 3+ ions formed during electroporation. Also to assess its practical applications value, a smartphone-integrated intelligent platform was successfully built and applied to detect Al 3+ in water samples, and satisfactory recoveries were attained, which powerfully proved that NPDM possesses a great practical potential for the visual detection of Al 3+ in environmental samples with the advantages of portability, simplicity, rapidity, low cost, and on-site sensing. Hence, according to the present results, we believe that more efforts can be devoted to the progress of ESIPT-active fluorogenic tweezers and helped to extend their practical application areas in the subsequent study.