AbstractSelectively tracking and quantifying Al3+ ions is a significant concern to the scientific communities. In the present article, an imine‐linkage electron donor‐acceptor system, DSAN, (E)‐5‐(diethylamino)‐2‐(((2‐hydroxy‐4‐nitrophenyl)imino)methyl)phenol has been introduced which shows Al3+ ions endows red light fluorogenicity which could be utilized for sequential and detection of Al3+ ions and picric acid (PA) in both solid and liquid phases. Upon addition of Al3+ ions into the DSAN solution, an orange‐red fluorescence is noticed at 604 nm caused by the formation of Al3+ ions chelated DSAN complex having detection and quantification limit 0.2 μM and 0.62 μM respectively in dimethylformamide (DMF) medium. The complex formation is found to be a 1 : 1 stoichiometric ratio as evident from Job's plot analysis. Also, the binding affinity value is found to be 3.24×104 M−1 demonstrating a high affinity of DSAN towards Al3+ ions. This orange‐red fluorescence of Al3+ ions chelated DSAN complex solution is quenched due to the introduction of PA. A super handy paper‐strips‐based detection tool also been fabricated utilizing DSAN which could be employed to track trace amounts of Al3+ ions in the solid state. The mechanism involved in the detection of Al3+ ions is elucidated by density functional theoretical analysis.