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The work introduces silica confinement of Tb(III) and Yb(III) complexes with p-sulfonatothiacalix[4]arene (TCAS) arisen from their doping into silica nanoparticles (51–60 nm) as the reason for efficient dual green–NIR luminescence. pH-regulated water solubility of the lanthanide complexes is highlighted as prerequisite for the balance between efficient doping of the complexes into silica nanoparticles...