Two hexanudear Ln(III) duster-based metal-organic frameworks (MOFs) (Ln = Tb or Eu) and a series of isomorphic bimetallic Ln(III)-MOFs have been synthesized by changing the ratio of Tb(III) and Eu(III) under solvothermal conditions. The excellent linear color tunability (from green to red) makes them suitable for barcode application. In addition, the anionic Ln(III)-MOFs exhibit superior uptake capacity toward methylene blue (MB+) by an ion exchange process, and its reversible adsorption performance makes 1 suitable for removal of organic dye MB+. The as-prepared anionic hexanuclear Ln(III) duster-based MOFs can serve as a multifunctional material for an optical and environmental area.