Developing intelligent supramolecular assemblies endowed with highly tunable optical properties has been a challenge. Herein, we demonstrate pH tolerant metal ion controlled highly tunable optical properties of a fluorescence quenched supramolecular assembly composed of sulfated-β-cyclodextrin (SβCD) templated acridine orange (AO+) aggregates by using an external stimulus, aluminium (Al3+), a well-known neurotoxic metal ion. The addition of Al3+ ion to the AO+-SβCD complex provides a strong screening effect, resisting the electrostatic interaction between the AO+ and SβCD host, which triggers significant changes in the absorption and fluorescence characteristics of the AO+-SβCD complex along with a favorable fluorescence turn-On response. Additionally, the fluorescence On-Off-On switching of AO+ activated by SβCD and Al3+ ion was successfully utilised to construct an uncommon supramolecular-based two-input IMPLICATION logic gate. Finally, we could also monitor the fluorescence On-Off-On switching events of AO+ in more complex live MCF-7 cancer cells, suggesting the potential of the current system in real-time monitoring of in-vivo biosensing and drug delivery applications.