<p>Tunable lanthanide supramolecular cascade panchromatic luminescence assembly was constructed by co-assembly of naphthylimidazolium picolinic acid (G₁)@Tb³⁺ complex, laponite (LP), diarylethene derivative, and Nile blue/Nile red with Rh800, which not only displayed the cascade energy transfer of light-harvesting from the optically adjustable rare-earth Tb³⁺ to Nile blue (energy transfer efficiency: 58%) or Nile red (75%), then to Rh800 (&gt;20%), leading to an ultra-large Stokes shift over 600 nm, but also showed the acid-base adjustable assembly and disassembly. Especially, the electrostatic interactions between LP and the positively charged G₁ effectively promote the green luminescence of Tb and the blue luminescence of G₁ in supramolecular assembly. Significantly, this lanthanide supramolecular assembly leverages the multi-component cascade energy transfer to create a powerful information security platform. By precisely tuning the ratio of donor G₁@Tb and acceptors Nile blue/Rh800, this assembly can generate tunable multi-color spectral outputs. This unique feature enables it to serve as multifunctional writing inks, facilitating switchable data logic encryption for multi-color information anti-counterfeiting, encoding information in ASCII format by embedding complex data within the multi-colored patterns and accurately read out via a simple scanning, and providing a convenient and efficient method for information storage and retrieval while ensuring high-level security.</p>